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Kanai, Yamato, Koji Hiraoka, Mutsuhiro Matsuyama, and Shiro Seki. "Chemically and Physically Cross-Linked Inorganic–Polymer Hybrid Solvent-Free Electrolytes." Batteries 9, no. 10 (September 26, 2023): 492. http://dx.doi.org/10.3390/batteries9100492.
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Safe, self-standing, all-solid-state batteries with improved solid electrolytes that have adequate mechanical strength, ionic conductivity, and electrochemical stability are strongly desired. Hybrid electrolytes comprising flexible polymers and highly conductive inorganic electrolytes must be compatible with soft thin films with high ionic conductivity. Herein, we propose a new type of solid electrolyte hybrid comprising a glass–ceramic inorganic electrolyte powder (Li1+x+yAlxTi2−xSiyP3−yO12; LICGC) in a poly(ethylene)oxide (PEO)-based polymer electrolyte that prevents decreases in ionic conductivity caused by grain boundary resistance. We investigated the cross-linking processes taking place in hybrid electrolytes. We also prepared chemically cross-linked PEO/LICGC and physically cross-linked poly(norbornene)/LICGC electrolytes, and evaluated them using thermal and electrochemical analyses, respectively. All of the obtained electrolyte systems were provided with homogenous, white, flexible, and self-standing thin films. The main ionic conductive phase changed from the polymer to the inorganic electrolyte at low temperatures (close to the glass transition temperature) as the LICGC concentration increased, and the Li+ ion transport number also improved. Cyclic voltammetry using [Li metal|Ni] cells revealed that Li was reversibly deposited/dissolved in the prepared hybrid electrolytes, which are expected to be used as new Li+-conductive solid electrolyte systems.
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Choi, Kyoung Hwan, Eunjeong Yi, Kyeong Joon Kim, Seunghwan Lee, Myung-Soo Park, Hansol Lee, and Pilwon Heo. "(Invited) Pragmatic Approach and Challenges of All Solid State Batteries: Hybrid Solid Electrolyte for Technical Innovation." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 988. http://dx.doi.org/10.1149/ma2023-016988mtgabs.
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For the growth of electric vehicle market, lithium-ion batteries (LIBS) used in the EVs still requires safety and reliability. Unfortunately, large-scale application of the LIBs is being challenged due to the fact that the use of flammable liquid electrolytes has caused safety issues such as leakage and fire explosion. In this respect, all-solid-state batteries (ASSBs) have been intensively studied to ensure the safety and mileage that are superior to the current LIBs. In terms of solid electrolytes, oxide electrolytes not only shows high ionic conductivity (10-4 ~ 10-3 S/cm) but also high mechanical strength to suppress surface dendrite formation. In addition, the oxide electrolytes possess advantages such as non-flammability, high thermal stability, and excellent electrochemical stability (~ 6 V), enabling high temperature/high voltage operations of oxide-based ASSBs. However, most of oxide materials require a sintering process at high temperatures to form a planar solid electrolyte. And a lack of flexibility results in non-uniform electrolyte/electrode contact in the battery, which makes it difficult to apply the rigid oxide electrolyte directly. On the other hand, solid polymer electrolytes have also been actively investigated due to no leakage, good electrolyte/electrode contact, easy processing, flexibility, and good film formability. However, the solid polymer electrolytes have critical disadvantages such as low ionic conductivity at room temperature and low thermal/mechanical stability, which precludes commercialization of solid polymer-based ASSBs despite their advantages. To overcome each disadvantages of oxide and polymer electrolytes, we developed hybrid electrolytes for improved ionic conductivity, easy processing, and formation of continuous electrolyte/electrode interface. In this presentation, pragmatic approach and current challenges related to solid batteries will be discussed including innovative manufacturing process. Hybrid electrolytes and their synergistic effect on the battery performance as a promissing solution will be presented [Fig. 1]
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Liao, Cheng Hung, Chia-Chin Chen, Ru-Jong Jeng, and Nae-Lih (Nick) Wu. "Application of Artificial Interphase on Ni-Rich Cathode Materials Via Hybrid Ceramic-Polymer Electrolyte in All Solid State Batteries." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 1050. http://dx.doi.org/10.1149/ma2023-0161050mtgabs.
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Among many cathode materials, nickel-rich LiNi0.83Co0.12Mn0.05O2 (NCM 831205) has been spotlighted as one of the most feasible candidates for next-generation LIBs because of its high discharge capacity (~200 mAh/g). However, NCM 831205 shows significant performance degradation, which is mostly attributed to cation mixing, surface side reactions, and intrinsic structural instability originating from the large volume changes during repeated cycling. Conventional lithium ion batteries (LIB) normally use flammable nonaqueous liquid electrolytes, resulting in a serious safety issue in use. In this respect, all-solid-state batteries (ASSB) are regarded as a fundamental solution to address the safety issue by using a solid state electrolyte in place of the conventional liquid one. This work employed lithium sulfonate (SO3Li) tethered polymer, obtained from sulfonation of commercial polymer, to serve as the artificial protective coating on the active NCM831205 of the cathode for ASSB based on hybrid PEO-ceramic solid electrolyte. The coating layer should prevent direct contact of electrolyte with the cathode, thus avoid the negative effects such as microcracks of NCM831205 and undesired CEI formation. The preparation of hybrid ceramic-polymer electrolyte through a solvent-free process. The hybrid electrolytes exhibit good flexibility and processability with respect to pure ceramic and pure PEO polymer electrolyte. It is demonstrated that the hybrid electrolytes can penetrate into cathode under 60°C, providing a good Li+ transfer channel inside the battery. Moreover, the sulfone based polymer protective coating could effectively improve the electrochemical stability of the NCM831205 without sacrificing the battery performance. Keywords: NCM831205, Artificial Polymer Coating, All-Solid-State Batteries
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LI, X. D., X. J. YIN, C. F. LIN, D. W. ZHANG, Z. A. WANG, Z. SUN, and S. M. HUANG. "INFLUENCE OF I2 CONCENTRATION AND CATIONS ON THE PERFORMANCE OF QUASI-SOLID-STATE DYE-SENSITIZED SOLAR CELLS WITH THERMOSETTING POLYMER GEL ELECTROLYTE." International Journal of Nanoscience 09, no. 04 (August 2010): 295–99. http://dx.doi.org/10.1142/s0219581x10006831.
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Thermosetting polymer gel electrolytes (TPGEs) based on poly(acrylic acid)-poly(ethylene glycol) (PAA-PEG) hybrid were prepared and applied to fabricate dye-sensitized solar cells (DSCs). N-methylpyrrolidone (NMP) and γ-butyrolactone (GBL) were used as solvents for liquid electrolytes and LiI and KI as iodide source, separately. The microstructure of PAA-PEG shows a well swelling ability in liquid electrolyte and excellent stability of the swollen hybrid. The TPGE was optimized in terms of the liquid electrolyte absorbency and ionic conductivity photovoltaic performance. Quasi-solid-state DSCs containing TPGE with optimized KI electrolyte show higher efficiency, voltage, fill factor, and lower photocurrent than those with LiI electrolyte. The related mechanism was discussed. A quasi-solid-state DSC fabricated with optimized polymer gel electrolyte obtained an overall energy conversion efficiency of 4.90% under irradiation of 100 mW/cm2 (AM1.5).
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Vargas-Barbosa, Nella Marie, Sebastian Puls, and Henry Michael Woolley. "Hybrid Material Concepts for Thiophosphate-Based Solid-State Batteries." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 984. http://dx.doi.org/10.1149/ma2023-016984mtgabs.
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Solid-state batteries (SSBs) could replace conventional lithium-ion batteries due to the possibility of increasing the energy density of the cells by using lithium metal as the anode material.[1] Among the many electrolyte candidates for lithium SSBs, the lithium thiophosphates are particularly interesting due to their high ionic conductivities at room temperature (>1 mS/cm). However, the (electro)chemical stability of these solid electrolytes is limited and not fully compatible with state-of-the-art high-potential cathode active materials[2] or the lithium metal anode.[3] At the cell level, the formation of interparticle voids between the various battery components (solid electrolyte, cathode active material, anode material, additives, decomposition interphases) hinder the net transport during cycling. To address the latter electro-chemo-mechanical challenges, we are exploring hybrid material approaches, in which we combine established materials (solid electrolytes, liquid electrolytes and/or polymer additives) with state-of-the-art cathode active materials and test their electrochemical performance in solid-state battery (half-)cells. Such cycling results are complimented by detailed electrochemical transport studies in symmetrical cells using DC polarization and electrochemical impedance spectroscopy, including transmission-line modeling. ex.situ chemically-specific spectroscopic methods are used to support our hypotheses and interpretation of the electrochemical results. Taken together, we attain a better picture on the positive (or negative) role hybrid materials play in SSBs. In this talk, we will showcase two hybrid systems, namely ionic liquid/thiophosphate lithium hybrid electrolytes and conductive polymers additives in NMC-based catholyte composites for Li6PS5Cl cells. The first part of the talk we will discuss the results in which we evaluate the performance of liquid electrolyte-solid electrolyte materials against lithium metal using galvanostatic electrochemical impedance spectroscopy. In the second part, we elucidate the partial ionic and electronic transport in polymer electrolyte-Li6PS5Cl-NMC catholytes as a function of polymer content using impedance spectroscopy and its effect in the cycling performance, both the stability as well as the magnitude of the discharge capacities. These systems serve as a good starting point for the further development and incorporation of hybrid materials in SSBs. Literature: [1] W. G. Zeier and J. Janek Nature Energy, 2016, 1, 16141. [2] G.F. Dewald, S. Ohno, M.A. Kraft, R. Kroever, P. Till, N.M. Vargas-Barbosa, J. Janek, W.G. Zeier Chem. Mater. 2019, 31, 8328. [3] L. M. Riegger, R. Schlem, J. Sann, W. G. Zeier, J. Janek, Angew. Chem. Int Ed 2021, 60, 6718. Figure 1
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Spencer Jolly, Dominic, Dominic L. R. Melvin, Isabella D. R. Stephens, Rowena H. Brugge, Shengda D. Pu, Junfu Bu, Ziyang Ning, et al. "Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries." Inorganics 10, no. 5 (April 26, 2022): 60. http://dx.doi.org/10.3390/inorganics10050060.
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Hybrid solid-state batteries using a bilayer of ceramic and solid polymer electrolytes may offer advantages over using a single type of solid electrolyte alone. However, the impedance to Li+ transport across interfaces between different electrolytes can be high. It is important to determine the resistance to Li+ transport across these heteroionic interfaces, as well as to understand the underlying causes of these resistances; in particular, whether chemical interphase formation contributes to giving high resistances, as in the case of ceramic/liquid electrolyte interfaces. In this work, two ceramic electrolytes, Li3PS4 (LPS) and Li6.5La3Zr1.5Ta0.5O12 (LLZTO), were interfaced with the solid polymer electrolyte PEO10:LiTFSI and the interfacial resistances were determined by impedance spectroscopy. The LLZTO/polymer interfacial resistance was found to be prohibitively high but, in contrast, a low resistance was observed at the LPS/polymer interface that became negligible at a moderately elevated temperature of 50 °C. Chemical characterization of the two interfaces was carried out, using depth-profiled X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry, to determine whether the interfacial resistance was correlated with the formation of an interphase. Interestingly, no interphase was observed at the higher resistance LLZTO/polymer interface, whereas LPS was observed to react with the polymer electrolyte to form an interphase.
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Spencer Jolly, Dominic, Dominic L. R. Melvin, Isabella D. R. Stephens, Rowena H. Brugge, Shengda D. Pu, Junfu Bu, Ziyang Ning, et al. "Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries." Inorganics 10, no. 5 (April 26, 2022): 60. http://dx.doi.org/10.3390/inorganics10050060.
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Hybrid solid-state batteries using a bilayer of ceramic and solid polymer electrolytes may offer advantages over using a single type of solid electrolyte alone. However, the impedance to Li+ transport across interfaces between different electrolytes can be high. It is important to determine the resistance to Li+ transport across these heteroionic interfaces, as well as to understand the underlying causes of these resistances; in particular, whether chemical interphase formation contributes to giving high resistances, as in the case of ceramic/liquid electrolyte interfaces. In this work, two ceramic electrolytes, Li3PS4 (LPS) and Li6.5La3Zr1.5Ta0.5O12 (LLZTO), were interfaced with the solid polymer electrolyte PEO10:LiTFSI and the interfacial resistances were determined by impedance spectroscopy. The LLZTO/polymer interfacial resistance was found to be prohibitively high but, in contrast, a low resistance was observed at the LPS/polymer interface that became negligible at a moderately elevated temperature of 50 °C. Chemical characterization of the two interfaces was carried out, using depth-profiled X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry, to determine whether the interfacial resistance was correlated with the formation of an interphase. Interestingly, no interphase was observed at the higher resistance LLZTO/polymer interface, whereas LPS was observed to react with the polymer electrolyte to form an interphase.
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Lee, Yan Ying, and Andre Weber. "Harmonization of Testing Procedures for All Solid State Batteries." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 340. http://dx.doi.org/10.1149/ma2023-022340mtgabs.
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All Solid State Batteries (ASSBs) with lithium-ion based conducting solid state electrolytes are considered the next generation high performance batteries. They enable high power densities due to their single ion conducting solid electrolyte, eliminating salt concentration gradients and related polarization losses in the cell, and ensuring an unrivalled level of safety due to their non-combustibility. Currently, a variety of ASSBs based on different solid state electrolytes such as polymers, thiophosphates, oxides and combinations thereof are being developed. One general problem with ASSBs is establishing and maintaining contact between the solid electrolyte and the active material phase during production and cycling, respectively. In conventional lithium-ion batteries (LiBs), this contact is ensured by the liquid state of the electrolyte, but in ASSBs, chemical expansion and contraction of the active material during lithiation and delithiation can detach this contact, resulting in decreased capacity due to the loss of active material. As a consequence, ASSBs are often operated under pressurized conditions, applying pressures significantly exceeding those in conventional LiBs. The same holds for the operating temperature window. Especially for polymer electrolyte-based ASSBs, they are often operated at higher temperatures to compensate for the low ionic conductivity of polymers at room temperature. With respect to cell testing, such operating requirements must be considered, and testing protocols are designed according to the individual requirements of the tested cell. This contribution aims to provide an overview of testing protocols for various types of ASSBs applied to different cells with polymer-, thiophosphate-, oxide-, and hybrid-electrolytes. These protocols will be compared with standardized testing routines for conventional LiBs. Based on this compilation, a harmonized testing procedure that covers the special requirements of the individual cell types and enables a fair comparison of different ASSBs is suggested. Additionally, examples of ASSB testing results will be discussed, taking into consideration the harmonization of different testing parameters.
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Villaluenga, Irune, Kevin H. Wujcik, Wei Tong, Didier Devaux, Dominica H. C. Wong, Joseph M. DeSimone, and Nitash P. Balsara. "Compliant glass–polymer hybrid single ion-conducting electrolytes for lithium batteries." Proceedings of the National Academy of Sciences 113, no. 1 (December 22, 2015): 52–57. http://dx.doi.org/10.1073/pnas.1520394112.
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Despite high ionic conductivities, current inorganic solid electrolytes cannot be used in lithium batteries because of a lack of compliance and adhesion to active particles in battery electrodes as they are discharged and charged. We have successfully developed a compliant, nonflammable, hybrid single ion-conducting electrolyte comprising inorganic sulfide glass particles covalently bonded to a perfluoropolyether polymer. The hybrid with 23 wt% perfluoropolyether exhibits low shear modulus relative to neat glass electrolytes, ionic conductivity of 10−4 S/cm at room temperature, a cation transference number close to unity, and an electrochemical stability window up to 5 V relative to Li+/Li. X-ray absorption spectroscopy indicates that the hybrid electrolyte limits lithium polysulfide dissolution and is, thus, ideally suited for Li-S cells. Our work opens a previously unidentified route for developing compliant solid electrolytes that will address the challenges of lithium batteries.
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Kirchberger, Anna Maria, Patrick Walke, and Tom Nilges. "Effect of Nanostructured Inorganic Ceramic Filler on Poly(ethylene oxide)-Based Solid Polymer Electrolytes." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 991. http://dx.doi.org/10.1149/ma2023-016991mtgabs.
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In view of the ongoing changes in energy science and technology, the possibilities of energy storage are getting increasingly important. In particular, storing electrical energy is more complex than with fossil fuels. Lithium-Ion batteries are the most commonly used media for energy storage, but they also have some safety-related problems: toxic decomposition products can leak out and the devices can catch fire. Research is underway to find alternatives to minimize this potential hazards. Great improvements in safety matters can be achieved by replacing liquid electrolytes with ceramic/polymer hybrid electrolytes. These hybrid electrolytes combine the advantages of polymer electrolytes with the benefits of inorganic ceramic fillers.1 Flexibility, good contact ability and in addition the good processability is provided through the polymer. The inorganic ceramic filler in contrast adds mechanical stability, opens new pathways for the Lithium-Ions and can enhance the stability of the electrolyte. Figure 1: different Lithium-ion pathways in ceramic/polymer hybrid electrolytes dependent on different filler amounts. 2 In this work the impact of the manufacturing method on the conductivity of a series of electrolytes was examined. Therefore, hot pressing, solution casting and electrospinning were tested. Also, different distribution methods for the particles in the material were tested to monitor the influence of agglomeration on the conductivity. The materials were characterized regarding the crystallinity using X-Ray diffraction, the surface and particle distribution was monitored with SEM/EDX, the thermal character was investigated using DSC, the conductivity was determined using impedance spectroscopy and the electrochemical behavior was tested using cyclic voltammetry. Furthermore, the Arrhenius equation was used to interpret the results of impedance spectroscopy regarding their activation energy. The addition of inorganic ceramic fillers leads to an enhancement of the ionic conductivity in PEO based electrolytes and increases processability and stability of the electrolyte. In this work conductivities of 10-5 S/cm were reached at room temperature. The performance of the electrolyte was increased above three orders of magnitude compared to a PEO electrolyte without inorganic ceramic fillers. Walke, P.; Kirchberger, A.; Reiter, F.; Esken, D.; Nilges, T., Effect of nanostructured Al2O3 on poly(ethylene oxide)-based solid polymer electrolytes. Zeitschrift für Naturforschung B 2021, 76 (10-12), 615-624. Chen, L.; Li, Y.; Li, S.-P.; Fan, L.-Z.; Nan, C.-W.; Goodenough, J. B., PEO/garnet composite electrolytes for solid-state lithium batteries: From “ceramic-in-polymer” to “polymer-in-ceramic”. Nano Energy 2018, 46, 176-184. Figure 1
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Ji, Xiaoyu, Yiruo Zhang, Mengxue Cao, Quanchao Gu, Honglei Wang, Jinshan Yu, Zi-Hao Guo, and Xingui Zhou. "Advanced inorganic/polymer hybrid electrolytes for all-solid-state lithium batteries." Journal of Advanced Ceramics 11, no. 6 (May 13, 2022): 835–61. http://dx.doi.org/10.1007/s40145-022-0580-8.
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AbstractSolid-state batteries have become a frontrunner in humankind’s pursuit of safe and stable energy storage systems with high energy and power density. Electrolyte materials, currently, seem to be the Achilles’ heel of solid-state batteries due to the slow kinetics and poor interfacial wetting. Combining the merits of solid inorganic electrolytes (SIEs) and solid polymer electrolytes (SPEs), inorganic/polymer hybrid electrolytes (IPHEs) integrate improved ionic conductivity, great interfacial compatibility, wide electrochemical stability window, and high mechanical toughness and flexibility in one material, having become a sought-after pathway to high-performance all-solid-state lithium batteries. Herein, we present a comprehensive overview of recent progress in IPHEs, including the awareness of ion migration fundamentals, advanced architectural design for better electrochemical performance, and a perspective on unconquered challenges and potential research directions. This review is expected to provide a guidance for designing IPHEs for next-generation lithium batteries, with special emphasis on developing high-voltage-tolerance polymer electrolytes to enable higher energy density and three-dimensional (3D) continuous ion transport highways to achieve faster charging and discharging.
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Mohanty, Debabrata, Shu-Yu Chen, and I.-Ming Hung. "Effect of Lithium Salt Concentration on Materials Characteristics and Electrochemical Performance of Hybrid Inorganic/Polymer Solid Electrolyte for Solid-State Lithium-Ion Batteries." Batteries 8, no. 10 (October 9, 2022): 173. http://dx.doi.org/10.3390/batteries8100173.
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Lithium-ion batteries are popular energy storage devices due to their high energy density. Solid electrolytes appear to be a potential replacement for flammable liquid electrolytes in lithium batteries. This inorganic/hybrid solid electrolyte is a composite of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, (poly(vinylidene fluoride-hexafluoro propylene) (PVDF-HFP) polymer and sodium superionic conductor (NASICON)-type Li1+xAlxTi2−x(PO4)3 (LATP) ceramic powder. The structure, morphology, mechanical behavior, and electrochemical performance of this composite solid electrolyte, based on various amounts of LiTFSI, were investigated. The lithium-ion transfer and conductivity increased as the LiTFSI lithium salt concentration increased. However, the mechanical strength apparently decreased once the percentage of LITFSI was over 60%. The hybrid electrolyte with 60% LiTFSI content showed high ionic conductivity of 2.14 × 10−4 S cm−1, a wide electrochemical stability window (3–6 V) and good electrochemical stability. The capacity of the Li|60% LiTFSI/PVDF-HFP/LATP| LiFePO4 solid-state lithium-metal battery was 103.8 mA h g−1 at 0.1 C, with a high-capacity retention of 98% after 50 cycles.
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Thangadurai, Venkataraman. "(Invited) Garnet Solid Electrolytes for Advanced All-Solid-State Li Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 47 (October 9, 2022): 1759. http://dx.doi.org/10.1149/ma2022-02471759mtgabs.
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These days, Li metal anode-based battery has been arisen as one of the key energy storage technologies due to its high theoretical energy density compared to conventional lithium and sodium ion-based batteries. The present Li-S batteries suffer due to Li dendrite formation and capacity decay due to polysulfide dissolution effect, because of organic electrolytes used in the current research. Solid state (ceramic) electrolytes are promising to prevent Li dendrite growth and polysulfide dissolution. Among different ceramic electrolytes garnet-type structure solid inorganic electrolytes are very promising because of its high lithium-ion conductivity and stability with elemental Li. However, the high interfacial resistance with the electrode is the major bottleneck for the practical use of ceramic electrolyte. Polymer and ceramic hybrid electrolytes exhibit low interfacial resistance. In this talk, we will present development of electrolytes for all-solid-state Li metal batteries.
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Thangadurai, Venkataraman. "(Invited) Lithium – Sulfur Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 545. http://dx.doi.org/10.1149/ma2022-024545mtgabs.
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These days, Li-S battery has been arisen as one of the key energy storage technologies due to its high theoretical energy density compared to conventional lithium and sodium ion-based batteries. The present Li-S batteries suffer due to Li dendrite formation and capacity decay due to polysulfide dissolution effect, due to organic electrolytes used in the current research. Solid state (ceramic) electrolytes are promising to prevent Li dendrite growth and polysulfide dissolution. Among different ceramic electrolytes garnet-type structure solid inorganic electrolytes are very promising because of its high lithium-ion conductivity and stability with elemental Li. However, the high interfacial resistance with the electrode is the major bottleneck for the practical use of ceramic electrolyte. Polymer and ceramic hybrid electrolytes exhibit low interfacial resistance. In this talk, we will present development of novel hybrid electrolytes for all-solid-state Li-S batteries, along with new methods to produce S cathodes with minimal polysulfide shuttle effect.
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Méry, Adrien, Steeve Rousselot, David Lepage, David Aymé-Perrot, and Mickael Dollé. "Limiting Factors Affecting the Ionic Conductivities of LATP/Polymer Hybrid Electrolytes." Batteries 9, no. 2 (January 28, 2023): 87. http://dx.doi.org/10.3390/batteries9020087.
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All-Solid-State Lithium Batteries (ASSLB) are promising candidates for next generation lithium battery systems due to their increased safety, stability, and energy density. Ceramic and solid composite electrolytes (SCE), which consist of dispersed ceramic particles within a polymeric host, are among the preferred technologies for use as electrolytes in ASSLB systems. Synergetic effects between ceramic and polymer electrolyte components are usually reported in SCE. Herein, we report a case study on the lithium conductivity of ceramic and SCE comprised of Li1.4Al0.4Ti1.6(PO4)3 (LATP), a NASICON-type ceramic. An evaluation of the impact of the processing and sintering of the ceramic on the conductive properties of the electrolyte is addressed. The study is then extended to Poly(Ethylene) Oxide (PEO)-LATP SCE. The presence of the ceramic particles conferred limited benefits to the SCE. These findings somewhat contradict commonly held assumptions on the role of ceramic additives in SCE.
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Zhang, L. X., Y. Z. Li, L. W. Shi, R. J. Yao, S. S. Xia, Y. Wang, and Y. P. Yang. "Electrospun Polyethylene Oxide (PEO)-Based Composite polymeric nanofiber electrolyte for Li-Metal Battery." Journal of Physics: Conference Series 2353, no. 1 (October 1, 2022): 012004. http://dx.doi.org/10.1088/1742-6596/2353/1/012004.
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Abstract Composite polymer electrolytes (CPEs) based on polyethylene oxide (PEO) offer manufacturing feasibility and outstanding mechanical flexibility. However, the low ionic conductivity of the CPEs at room temperature, as well as the poor mechanical properties, have hindered their commercialization. In this work, Solid-state electrolytes based on polyethylene oxide (PEO) with and without fumed SiO2 (FS) nanoparticles are prepared by electrostatic spinning process. The as-spun PEO hybrid nanofiber electrolyte with 6.85 wt% FS has a relatively high lithium ion conductivity and electrochemical stability, which is 4.8 × 10-4 S/cm and up to 5.2 V vs. Li+/Li, respectively. Furthermore, it also shows a higher tensile strength (2.03 MPa) with % elongation at break (561.8). Due to the superior electrochemical and mechanical properties, it is promising as high-safety and all-solid-state polymer electrolyte for advanced Li-metal battery.
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Zhai, Yanfang, Wangshu Hou, Zongyuan Chen, Zhong Zeng, Yongmin Wu, Wensheng Tian, Xiao Liang, et al. "A hybrid solid electrolyte for high-energy solid-state sodium metal batteries." Applied Physics Letters 120, no. 25 (June 20, 2022): 253902. http://dx.doi.org/10.1063/5.0095923.
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Exploring solid electrolytes with promising electrical properties and desirable compatibility toward electrodes for safe and high-energy sodium metal batteries remains a challenge. In this work, these issues are addressed via an in situ hybrid strategy, viz., highly conductive and thermally stable 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide is immobilized in nanoscale silica skeletons to form ionogel via a non-hydrolytic sol-gel route, followed by hybridizing with polymeric poly(ethylene oxide) and inorganic conductor Na3Zr2Si2PO12. Such hybrid design yields the required solid electrolyte, which shows not only a stable electrochemical stability window of 5.4 V vs Na/Na+ but also an extremely high ionic conductivity of 1.5 × 10−3 S cm−1 at 25 °C, which is demonstrated with the interacted and monolithic structure of the electrolyte by SEM, XRD, thermogravimetric (TG), and XPS. Moreover, the capabilities of suppressing sodium metal dendrite growth and enabling high-voltage cathode Mg-doped P2-type Na0.67Ni0.33Mn0.67O2 are verified. This work demonstrates the potential to explore the required solid electrolytes by hybridizing an in situ ionogel, a polymer, and an inorganic conductor for safe and high-energy solid-state sodium metal batteries.
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Ryu, Kun, Kyungbin Lee, Hyun Ju, Jinho Park, Ilan Stern, and Seung Woo Lee. "Ceramic/Polymer Hybrid Electrolyte with Enhanced Interfacial Contact for All-Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2621. http://dx.doi.org/10.1149/ma2022-0272621mtgabs.
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All solid-state lithium batteries (ASSLBs) with a high energy density are challenging, yet desired by the rising energy demands. Its intrinsic safety of solid-state electrolytes (SSEs) compared to flammable liquid electrolytes makes ASSLBs a modern-day necessity. NASICON-type Li1.5Al0.5Ge1.5P3O12 (LAGP) has high ionic conductivity, high stability against air and water, and a wide electrochemical window. However, the application of LAGP is significantly hindered by its slow interfacial kinetics and brittle nature. In addition, the ionic conductivity of LAGP is relatively low at room temperature compared to that obtained at elevated temperatures. In our study, LAGP was incorporated into a polymer matrix to accelerate charge transport at the electrode-electrolyte interface to form LAGP-poly-DOL (LAGP-pDOL) hybrid electrolyte. The in-situ cationic ring-opening polymerization of DOL decreases the interfacial contact impedance and improves the mechanical properties of the SSE. LAGP-pDOL electrolyte exhibits prolonged cycle stability in symmetric cells (> 200 h) and in Li|LiFePO4 full cells (99% retention after 50 cycles) at room temperature. This study demonstrates the effective utilization of conductive polymer matrix into LAGP to enhance mechanical strength, interfacial contact, and room temperature electrochemical performance.
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Giffin, Guinevere A., Mara Goettlinger, Hendrik Bohn, Simone Peters, Mario Weller, Alexander Naßmacher, Timo Brändel, and Alex Friesen. "Development of a Polymer-Based Silicon-NMC Solid-State Cell." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 373. http://dx.doi.org/10.1149/ma2023-022373mtgabs.
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Solid-state batteries are seen as the next generation of battery technology with the promise of high energy density and improved safety as compared to conventional lithium-ion batteries. To achieve these goals, high-capacity negative electrodes, e.g., silicon or lithium, need to be combined with high capacity and high voltage positive electrodes, e.g., Ni-rich NMC. This combination of active materials provides a number of significant challenges for the solid-state electrolyte. If silicon is used as the anode active material, significant volume changes during lithiation/delithiation occur. These volume changes lead to a variety of problems including irreversible loss of lithium and eventual disintegration of the electrodes, resulting in capacity fade. Therefore, the electrolyte must be sufficiently elastic to buffer these changes. If Ni-rich NMC is used as a cathode active material, then the electrolyte must be stable at voltages up to at least 4.2 V. There are currently few, if any, electrolyte solutions that can address these challenges simultaneously. In the ASTRABAT project, a silicon-NMC solid-state cell has been developed based on two tailored polymer electrolytes, which allows the specific challenges of each cell compartment to be addressed separately. A vinylidene fluoride copolymer-based electrolyte has been developed for use as a catholyte and a hybrid inorganic-organic polymer electrolyte as the anolyte. This work will report a characterization of both electrolytes, along with their electrochemical performance in solid-state half-cells and full-cells.
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Babkova, Tatiana, Rudolf Kiefer, and Quoc Bao Le. "Hybrid Electrolyte Based on PEO and Ionic Liquid with In Situ Produced and Dispersed Silica for Sustainable Solid-State Battery." Sustainability 16, no. 4 (February 19, 2024): 1683. http://dx.doi.org/10.3390/su16041683.
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This work introduces the synthesis of hybrid polymer electrolytes based on polyethylene oxide (PEO) and electrolyte solution bis(trifluoromethane)sulfonimide lithium salt/ionic liquid 1-ethyl-3-methyl-imidazolium bis(trifluoromethylsulfonyl)imide (LiTFSI/EMIMTFSI) with in situ produced and dispersed silica particles by the sol–gel method. Conventional preparation of solid polymer electrolytes was followed by desolvation of lithium salt in a polymer matrix of PEO, which, in some cases, additionally contains plasticizers. This one-pot synthesis is an alternative route for fabricating a solid polymer electrolyte for solid-state batteries. The presence of TFSI- reduces the crystallinity of the PEO matrix (plasticizing effect), increases the dissociation and solubility of LiTFSI in the PEO matrix because of a highly delocalized charge distribution, and reveals excellent thermal, chemical, and electrochemical stability. Tetraethylorthosilicate (TEOS) was chosen due to the slow reaction rate, with the addition of (3-glycidyoxypropyl)trimethoxysilane (GLYMO), which contributes to the formation of a silica network. FTIR studies confirmed the interactions between the silica, the polymer salt, and EMIMTFSI. Impedance spectroscopy measurements were performed in a wide range of temperatures from 25 to 70 °C. The electrochemical performance was explored by assembling electrolytes in LiCoO2 (LCO), NMC(811), and LiFePO4 (LFP) coin half-cells. The HPEf15 shows a discharge capacity of 143 mA/g for NMC(811) at 0.1 C, 134 mA/g for LCO, and 139 mA/g for LFP half-cells at 0.1 C and 55 °C. The LFP half-cell with a discharge capacity of 135 mA/g at 0.1 C (safety potential range of 2.8 to 3.8) obtained a cyclability of 97.5% at 55 °C after 100 cycles. Such a type of electrolyte with high safety and good electrochemical performance provides a potential approach for developing a safer lithium-ion battery.
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De Cachinho Cordeiro, Ivan Miguel, Ao Li, Bo Lin, Daphne Xiuyun Ma, Lulu Xu, Alice Lee-Sie Eh, and Wei Wang. "Solid Polymer Electrolytes for Zinc-Ion Batteries." Batteries 9, no. 7 (June 27, 2023): 343. http://dx.doi.org/10.3390/batteries9070343.
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To date, zinc-ion batteries (ZIBs) have been attracting extensive attention due to their outstanding properties and the potential to be the solution for next-generation energy storage systems. However, the uncontrollable growth of zinc dendrites and water-splitting issues seriously restrict their further scalable application. Over the past few years, solid polymer electrolytes (SPEs) have been regarded as a promising alternative to address these challenges and facilitate the practical advancement of zinc batteries. In this review, we revisit the research progress of SPEs applied in zinc batteries in the past few years and focus on introducing cutting-edge polymer science and technologies that can be utilised to prepare advanced SPEs for high-performance zinc batteries. The operating mechanism of SPEs and the functions of polymers are summarised. To highlight the polymer’s functions, SPEs are categorised into three types, homogenous polymer SPEs, hybrids polymer SPEs, and nanocomposites SPEs, which are expected to reveal the roles and principles of various polymers in zinc batteries. This review presents the current research progress and fundamental mechanisms of polymer-based SPEs in zinc batteries, outlines the challenging issues encountered, and proposes potential solutions for future endeavours.
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Pham, Quoc-Thai, Badril Azhar, and Chorng-Shyan Chern. "Novel Acrylonitrile-Based Polymers for Solid–State Polymer Electrolyte and Solid-State Lithium Ion Battery." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 160. http://dx.doi.org/10.1149/ma2022-012160mtgabs.
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Rechargeable lithium-ion batteries (LIBs) involving lithium metal oxides, liquid electrolyte and graphite have been widely used in portable electronic devices due to their relatively high energy density and long cycle life. These desirable features make LIBs very attractive as the power source for electronic devices, hybrid electric vehicles (HEVs) and electric vehicles (EVs) applications [1, 2]. For future EV applications, higher energy density of LIBs up to 360 Wh kg-1 is required. Currently, the energy density of the state-of-the-art LIBs using conventional graphite anode, LiFePO4 (denoted as LFP) or LiNi0.5Co0.2Mn0.3O2 (NCM523) cathodes and 1-1.2 M LiPF6 in organic carbonate electrolytes provide practically achievable energy densities of up to around 200-260 Wh kg−1 [3]. When commercial graphite anodes are used, LiNi0.8Co0.15Al0.05O2 (NCA), LiNi0.8Co0.1Mn0.1O2 (NCM811), LiNi0.5Mn1.5O4 (LNMO) and LiNiPO4 (LNP) cathode based batteries with high-voltage provide energy densities of 354, 338, 351 and 414 Wh kg-1, respectively. However, LIBs using these high-voltage cathode materials and the organic carbonate electrolytes exhibit quite low thermal stability and tend to catch fire or even explode when abnormal charge/discharge cycling or accidental penetration of cells occurs, which greatly limits the automotive applications. When replacing graphite with a Li metal anode, the energy densities of all battery systems can be enhanced significantly due to the highest theoretical specific energy density (3860 mAh g-1) among all anode materials for rechargeable LIBs. Nevertheless, commercial LIBs are prone to cause safety problems due to the safety concern arising from Li dendrite growth in liquid organic electrolytes [4-6]. The promising solid-state LIBs offer high thermal stability (i.e., low risk in catching fire), high energy density, wide electrochemical stability window and less environmental impact. A competent electrolyte is the key component of solid-state LIBs. The solid-state electrolyte materials are mainly classified as solid polymer electrolytes (SPEs), inorganic solid electrolytes (ISEs), and organic/inorganic composite electrolytes. ISEs include oxide-based and sulfide-based materials [7, 8], which show very high ionic conductivity (10-2 – 10-3 S cm-1). Furthermore, the lithium ion transference number is close to 1. However, the major limitation factors of practical solid-state LIB applications are the large interfacial impedance between electrode and ISE and the difficulty of processing [9]. Considering processability, mechanical flexibility, interfacial compatibility and electrochemical stability, one prefers SPEs to the inorganic ceramic electrolytes. Nevertheless, SPEs have low ion conductivities (10−7 − 10−5 S cm−1 near room temperature) and most of the Li+ transference numbers are lower than 0.5 [10, 11]. The major requirements for SPEs include high ionic conductivity and transference number at room temperature, wide electrochemical potential window, high mechanical strength and excellent thermal stability. However, the ion conductivity is the most important (> 10-4 S cm-1 at room temperature desired) and should be considered first. The coordinating groups of a good polymeric host are expected to interact with Li+ and facilitate dissociation. In this study, we prepared various novel acrylonitrile-based polymers (e.g., acrylonitrile/acrylate copolymer and polymer with two pendant groups b-cyano ethyl ether (-O-CH2CH2-CN) sulfonate alkyl ether (-O-(CH2)3SO3Li). The corresponding SPEs comprising acrylonitrile-based polymer and ca. 50 wt.% lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) with high ionic conductivity (up to 10-3 S cm-1) at room temperature, high ion transfer number (up to 0.45) and large electrochemical potential window (oxidation stability > 5 V vs. Li+/Li) achieved. The selected SPEs were used as the separator in solid-state batteries with LiFePO4 as the cathode and Li foil as the anode; and long-term cycle stability of solid-state LIB was achieved. The polymers and corresponding SPEs were characterized by using DSC, SEM, XRD and FTIR measurements. Ionic conductivities of SPEs were determined from electrochemical impedance spectroscopy results. The linear sweep voltammetry technique was adopted to measure the oxidation stability window of SPE, and the Evans-Vincent-Bruce method was used to determined ion transfer number. References [1] J.B. Goodenough, Energy Environ. Sci. 7 (2014) 14−18. [2] M. Armand, et al., Nature 451 (2008) 652-657. [3] F. Wu, et al., Chem Soc Rev 49 (2020) 1569-1614. [4] Q. Wang, et at., J Power Sources 208 (2012) 210-224. [5] A.W. Golubkov, et al., RSC Adv 5 (2015) 57171-57186. [6] Z. Wang, et al. Nat Energy 3, (2018) 227–235. [7] L. Fan, et al., Adv. Energy Mater. 2018, 8, 1702657. [8] G. Kim, et al., J Power Sources 282 (2015) 299-322. [9] P. Knauth, Solid State Ion 180 (2009) 911-916. [10] C. Ma, et al., J Power Sources 2016; 317 :103–11. [11] N.K. Karan, et al., Solid State Ion 179 (2008) 689–696. Figure 1
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Falco, Marisa, Gabriele Lingua, Silvia Porporato, Ying Zhang, Mingjie Zhang, Matteo Gastaldi, Francesco Gambino, et al. "An Overview on Polymer-Based Electrolytes with High Ionic Mobility for Safe Operation of Solid-State Batteries." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 604. http://dx.doi.org/10.1149/ma2023-024604mtgabs.
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Liquid electrolytes used in commercial Li-ion batteries are generally based on toxic volatile and flammable organic carbonate solvents, thus raising safety concerns in case of thermal runaway. The most striking solution at present is to switch on all solid-state designs exploiting polymer materials, films, ceramics, low-volatile, green additives, etc. The replacement of liquids component with low-flammable solids is expected to improve the safety level of the device intrinsically. Moreover, a solid-state configuration is expected to guarantee improved energy density systems. However, low ionic conductivity, low cation transport properties and issues in cell manufacturing processes must be overcome [1]. Electrochemical performance in lab-scale devices can be readily improved using different RTILs or specific low-volatile additives. Here, an overview is offered of the recent developments in our labs on innovative polymer-based electrolytes allowing high ionic mobility, particularly attractive for safe, high-performing, solid-state Li-metal batteries, and obtained by different techniques, including solvent-free UV-induced photopolymerization. Cyclic voltammetry and galvanostatic charge/discharge cycling coupled with electrochemical impedance spectroscopy exploiting different electrode materials (e.g., LFP, Li-rich NMC, LNMO, Si/C) demonstrate specific capacities approaching theoretical values even at high C-rates and stable operation for hundreds of cycles at ambient temperature [2,3]. Direct polymerization procedures on top of the electrode films are also used to obtain an intimate electrode/electrolyte interface and full active material utilization in both half and full-cell architectures. In addition, results of composite hybrid polymer electrolytes [4] and new single-ion conducting polymers [5] are shown, specifically developed to attain improved ion transport and high oxidation stability for safe operation with high voltage electrodes even at ambient conditions. References [1] Ferrari, S.; Falco, M.; Muñoz-García, A.B.; Bonomo, M.; Brutti, S.; Pavone, M.; Gerbaldi, C. Solid-State Post Li Metal Ion Batteries: A Sustainable Forthcoming Reality? Adv. Energy Mater. 2021, 11, 2100785. [2] Falco, M.; Simari, C.; Ferrara, C.; Nair, J.R.; Meligrana, G.; Nicotera, I.; Mustarelli, P.; Winter, M.; Gerbaldi, C. Understanding the Effect of UV-Induced Cross-Linking on the Physicochemical Properties of Highly Performing PEO/LiTFSI-Based Polymer Electrolytes. Langmuir 2019, 35, 8210-8219. [3] Lingua, G.; Falco, M.; Stettner, T.; Gerbaldi, C.; Balducci, A. Enabling safe and stable Li metal batteries with protic ionic liquid electrolytes and high voltage cathodes. J. Power Sources 2021, 481, 228979. [4] Falco, M.; Castro, L.; Nair, J.R.; Bella, F.; Bardé, F.; Meligrana, G.; Gerbaldi, C. UV-Cross-Linked Composite Polymer Electrolyte for High-Rate, Ambient Temperature Lithium Batteries. ACS Appl. Energy Mater. 2019, 2 1600-1607. [5] Lingua, G.; Grysan, P.; Vlasov, P.S.; Verge, P.; Shaplov, A.S.; Gerbaldi, C. Unique Carbonate-Based Single Ion Conducting Block Copolymers Enabling High-Voltage, All-Solid-State Lithium Metal Batteries. Macromolecules, 2021, 54, 6911-6924. Acknowledgements The Si-DRIVE project has received funding from the EU's Horizon 2020 research and innovation program under GA 814464. The PSIONIC project has received funding from the European Union's Horizon Europe Research and Innovation Programme under Grant Agreement N. 101069703.
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Kuppusamy, Hari Gopi, Prabhakaran Dhanasekaran, Niluroutu Nagaraju, Maniprakundil Neeshma, Baskaran Mohan Dass, Vishal M. Dhavale, Sreekuttan M. Unni, and Santoshkumar D. Bhat. "Anion Exchange Membranes for Alkaline Polymer Electrolyte Fuel Cells—A Concise Review." Materials 15, no. 16 (August 15, 2022): 5601. http://dx.doi.org/10.3390/ma15165601.
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Solid anion exchange membrane (AEM) electrolytes are an essential commodity considering their importance as separators in alkaline polymer electrolyte fuel cells (APEFC). Mechanical and thermal stability are distinguished by polymer matrix characteristics, whereas anion exchange capacity, transport number, and conductivities are governed by the anionic group. The physico-chemical stability is regulated mostly by the polymer matrix and, to a lesser extent, the cationic head framework. The quaternary ammonium (QA), phosphonium, guanidinium, benzimidazolium, pyrrolidinium, and spirocyclic cation-based AEMs are widely studied in the literature. In addition, ion solvating blends, hybrids, and interpenetrating networks still hold prominence in terms of membrane stability. To realize and enhance the performance of an alkaline polymer electrolyte fuel cell (APEFC), it is also necessary to understand the transport processes for the hydroxyl (OH−) ion in anion exchange membranes. In the present review, the radiation grafting of the monomer and chemical modification to introduce cationic charges/moiety are emphasized. In follow-up, the recent advances in the synthesis of anion exchange membranes from poly(phenylene oxide) via chloromethylation and quaternization, and from aliphatic polymers such as poly(vinyl alcohol) and chitosan via direct quaternization are highlighted. Overall, this review concisely provides an in-depth analysis of recent advances in anion exchange membrane (AEM) and its viability in APEFC.
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Sankara Raman, Ashwin, Samik Jhulki, Billy Johnson, Aashray Narla, and Gleb Yushin. "Facile in-Situ Polymerized Polymer Electrolytes in All Solid-State Lithium-Ion Batteries." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 316. http://dx.doi.org/10.1149/ma2022-023316mtgabs.
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With the push towards renewable energy sources and “green” technologies, lithium-ion batteries (LIBs) have proven to be necessary across multiple technological realms, the biggest of which is currently the electric vehicle (EV) and grid storage markets. But the popular choice of liquid organic electrolytes in LIBs suffers from safety concerns, which motivated significant innovations in safer solid-state electrolytes. Among them, solid polymer electrolytes (SPEs) have shown great potential due to their processability, flexibility and tunability of physical properties. The past decade has seen rapid evolution in the development of SPE LIBs, but most of them still stand inadequate. SPEs are typically processed either by using solvents, or by using them in their solid state, to blend with the active electrode materials. While these systems are often subject to additional compression to promote continuous electrolyte-electrode interface, they still suffer from the almost unavoidable formations of voids, and inhomogeneous contact between the active materials and the SPEs. Furthermore, most of these processes require excessive amounts of SPEs, and yet result in a large interfacial resistance. Here we introduce a novel one-step manufacturing strategy for polymer electrolytes in solvent-free SPE LIBs. The process involves in-situ polymerization of a liquid-monomer precursor directly infiltrated into a dry jelly roll or individual electrodes to form SPE cells. Our microscopy and FIB experiments confirmed a near-perfect polymer infiltration in porous cathodes, while electro-chemical tests confirmed excellent characteristics of cathode-electrolyte interfaces. The cycling performance of lithium iron phosphate (LFP) half cells using thus produced and infiltrated SPE showed very good stability and columbic efficiency. In addition to single-ion conductive SPEs, we tested hybrid SPE systems where Li salts were added into the single-ion conductive SPEs to improve rate and capacity utilization.
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Shah, Vaidik, and Yong Lak Joo. "Rationally Designed in-Situ Gelled Polymer-Ceramic Hybrid Electrolyte Enables Superior Performance and Stability in Quasi-Solid-State Lithium-Sulfur Batteries." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 535. http://dx.doi.org/10.1149/ma2023-024535mtgabs.
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Despite boasting giant leaps in performance improvement over the years, the current commercial standard, Li-ion batteries, are fast approaching their theoretical limits. Meanwhile, Lithium-Sulfur (Li-S) batteries offering ultra-high theoretical energy density (～2600 Whkg-1), cost-effectiveness, and nontoxicity are being seen as promising alternatives. Despite their plentiful advantages, the practicality of Li-S batteries has been largely stymied by several challenges: a) deleterious polysulfide dissolution and ‘shuttle effect’, b) significant volume change of S cathodes during cycling, c) safety concerns with flammable traditional glyme-based electrolyte, and d) the instability of Li anode. To mitigate these challenges, researchers have explored all-solid-state electrolytes, but their poor Li-ion conductivity, high interfacial impedance, and need for expensive, exotic materials and complex fabrication procedures severely limit their practical application. To overcome these challenges, we propose an in-situ gelled polymer-ceramic hybrid silsesquioxane-based electrolyte system. The gelled matrix, thermally crosslinked post cell fabrication, immobilizes the glyme-based liquid electrolyte and exhibits high liquid-like ionic conductivities (1.03 mS.cm-1), low interfacial impedance, and high oxidative potential (>4.5V vs. Li/Li+) . In this study, in addition to vastly decreased flammability, we report superior Li-ion conductivity compared to state-of-art solid-state Li-S electrolytes. This high ionic conductivity translated to a significantly improved specific capacity of 1050 mAh.gS-1 at 0.2 C, elevated Coulombic efficiencies (>98.5%), and elevated rate kinetics. The gelled electrolytes exhibited stable cycling in a large temperature range (-10oC - 60 oC). Moreover, polysulfide permeation studies and subsequent DFT calculations revealed that the gelled electrolyte exhibited strong chemical absorptivity to lithium polysulfides due to the polar silsesquioxane core, which translated to superior capacity retention (>80% over 200 cycles). Further, post- mortem XPS characterization studies revealed the formation of stable SEI at the anode and cathode, and SEM of cycled anodes showed reduced dendritic formations. Finally, the electrolyte was tested in practical pouch cell architecture, and the cells demonstrated excellent reliability even under mechanical stress. This work successfully reports a robust, rationally designed gelled electrolyte system for developing safe and high-performance quasi-solid state Li-S batteries.
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Okos, Alexandru, Cristina Florentina Ciobota, Adrian Mihail Motoc, and Radu-Robert Piticescu. "Review on Synthesis and Properties of Lithium Lanthanum Titanate." Materials 16, no. 22 (November 8, 2023): 7088. http://dx.doi.org/10.3390/ma16227088.
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The rapid development of portable electronic devices and the efforts to find alternatives to fossil fuels have triggered the rapid development of battery technology. The conventional lithium-ion batteries have reached a high degree of sophistication. However, improvements related to specific capacity, charge rate, safety and sustainability are still required. Solid state batteries try to answer these demands by replacing the organic electrolyte of the standard battery with a solid (crystalline, but also polymer and hybrid) electrolyte. One of the most promising solid electrolytes is Li3xLa2/3−xTiO3 (LLTO). The material nevertheless presents a set of key challenges that must be resolved before it can be used for commercial applications. This review discusses the synthesis methods, the crystallographic and the ionic conduction properties of LLTO and the main limitations encountered through a number of selected studies on this material.
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Lin, Ruifan, Yingmin Jin, Yumeng Li, Xuebai Zhang, and Yueping Xiong. "Recent Advances in Ionic Liquids—MOF Hybrid Electrolytes for Solid-State Electrolyte of Lithium Battery." Batteries 9, no. 6 (June 6, 2023): 314. http://dx.doi.org/10.3390/batteries9060314.
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Li-ion batteries are currently considered promising energy storage devices for the future. However, the use of liquid electrolytes poses certain challenges, including lithium dendrite penetration and flammable liquid leakage. Encouragingly, solid electrolytes endowed with high stability and safety appear to be a potential solution to these problems. Among them, ionic liquids (ILs) packed in metal organic frameworks (MOFs), known as ILs@MOFs, have emerged as a hybrid solid-state material that possesses high conductivity, low flammability, and strong mechanical stability. ILs@MOFs plays a crucial role in forming a continuous interfacial conduction network, as well as providing internal ion conduction pathways through the ionic liquid. Hence, ILs@MOFs can not only act as a suitable ionic conduct main body, but also be used as an active filler in composite polymer electrolytes (CPEs) to meet the demand for higher conductivity and lower cost. This review focuses on the characteristic properties and the ion transport mechanism behind ILs@MOFs, highlighting the main problems of its applications. Moreover, this review presents an introduction of the advantages and applications of Ils@MOFs as fillers and the improvement directions are also discussed. In the conclusion, the challenges and suggestions for the future improvement of ILs@MOFs hybrid electrolytes are also prospected. Overall, this review demonstrates the application potential of ILs@MOFs as a hybrid electrolyte material in energy storage systems.
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Aruchamy, Kanakaraj, Subramaniyan Ramasundaram, Sivasubramani Divya, Murugesan Chandran, Kyusik Yun, and Tae Hwan Oh. "Gel Polymer Electrolytes: Advancing Solid-State Batteries for High-Performance Applications." Gels 9, no. 7 (July 21, 2023): 585. http://dx.doi.org/10.3390/gels9070585.
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Gel polymer electrolytes (GPEs) hold tremendous potential for advancing high-energy-density and safe rechargeable solid-state batteries, making them a transformative technology for advancing electric vehicles. GPEs offer high ionic conductivity and mechanical stability, enabling their use in quasi-solid-state batteries that combine solid-state interfaces with liquid-like behavior. Various GPEs based on different materials, including flame-retardant GPEs, dendrite-free polymer gel electrolytes, hybrid solid-state batteries, and 3D printable GPEs, have been developed. Significant efforts have also been directed toward improving the interface between GPEs and electrodes. The integration of gel-based electrolytes into solid-state electrochemical devices has the potential to revolutionize energy storage solutions by offering improved efficiency and reliability. These advancements find applications across diverse industries, particularly in electric vehicles and renewable energy. This review comprehensively discusses the potential of GPEs as solid-state electrolytes for diverse battery systems, such as lithium-ion batteries (LiBs), lithium metal batteries (LMBs), lithium–oxygen batteries, lithium–sulfur batteries, zinc-based batteries, sodium–ion batteries, and dual-ion batteries. This review highlights the materials being explored for GPE development, including polymers, inorganic compounds, and ionic liquids. Furthermore, it underscores the transformative impact of GPEs on solid-state batteries and their role in enhancing the performance and safety of energy storage devices.
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Toghyani, Somayeh, Florian Baakes, Ningxin Zhang, Helmut Kühnelt, Walter Cistjakov, and Ulrike Krewer. "(Digital Presentation) Model-Assisted Design of Oxide-Based All-Solid-State Li-Batteries with Hybrid Electrolytes for Aviation." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 484. http://dx.doi.org/10.1149/ma2022-024484mtgabs.
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There is a growing interest in the sustainability of the aviation industry sector over the past years due to the environmental issues associated with traditional aviation engines. Electric and hybrid aircrafts are considered promising technologies for reducing fuel consumption and enhancing system efficiency [1]. However, electrical energy storage systems require a higher capacity-to-weight ratio than today’s Li-ion batteries to fulfil the high demands in this area. Safety restrictions imposed by liquid electrolytes motivate the development of next-generation chemistries, such as oxide-based all-solid-state batteries (ASSB) for aviation, which have non-flammable electrolytes [2]. This option is investigated in the context of the IMOTHEP European project that aims at identifying promising hybrid aircraft configurations and studying the associated technology. However, the major drawbacks of oxide-based solid electrolytes are weak contact between electrode and electrolyte interface, low mechanical flexibility, and high density, which limit their use for high gravimetric energy density applications. To mitigate the aforementioned concerns, the solid polymer composite electrolytes approach could be applied, where oxides are mixed with polymer electrolytes [3]. Designing an optimum cell without ion transport limitations using experimental investigations is time- as well as resource-intensive due to the large number of iterations in production and evaluation required to achieve a well-performing design. Physics-based modelling is able to create a platform that can directly assess the impact of cell structure on battery performance and provide knowledge concerning limiting processes within the cell. Therefore, we here present the first study that combines a pseudo-two-dimensional model for the model-assisted evaluation of Li-ASSB with various hybrid electrolytes and single-ion conductor electrolytes with an evolutionary algorithm to identify optimum cell designs to reach a higher gravimetric energy density (see Fig. 1-a). To this end, we first compared the performance of several hybrid electrolytes with their experimental properties, to identify which electrolyte performs well with present technology and which has the potential to become an attractive alternative in the future. Our findings reveal that based on available ASSB technology, single ion-conducting electrolytes cannot achieve a higher gravimetric energy density than hybrid electrolytes at low current rates due to their high density, as shown in Fig. 1-b. ASSB based on 12.7 vol% of garnet Li6.4La3Zr1.4Ta0.6O12 (LLZTO) is the best option based on present manufacturing constraints. Furthermore, our study revealed that hybrid electrolytes based on 10 wt% of Li1.3Al0.3Ti1.7(PO4)3 (LATP) could be promising for future aircraft if researchers succeed to decrease its electrolyte thickness and chemical stability in contact with lithium metal anode. Further, sensitivity analyses enabled us to identify that the cathode thickness and volume fraction of cathode materials are critical parameters for the cell design of ASSB. Therefore, we applied a global optimisation to enhance gravimetric energy density by changing these two electrode design parameters. After optimisation, gravimetric and volumetric energy densities of 618 Wh kg-1 and 1251 Wh L-1 for 0.1C discharge are achieved, respectively, indicating that the cell with the optimal electrode design could meet the mission demand in the aviation industry with a gravimetric energy density of 500 Wh kg-1 and volumetric energy density of 1000 Wh L-1. In conclusion, the findings of this study show that our physics-based modelling in conjunction with an optimisation algorithm predicts the optimal composition of ASSB for a given constraint and thus supports the time- and cost-effective development of batteries that fulfil mission requirements, e.g. in the aviation sector. This work is conducted in the frame of the project IMOTHEP (Investigation and Maturation of Technologies for Hybrid Electric Propulsion), which has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 875006 IMOTHEP. References: M. Tariq, A. I. Maswood, C. J. Gajanayake, and A. K. Gupta, IECON Proc. (Industrial Electron. Conf. 4429 (2016). J. Hoelzen, Y. Liu, B. Bensmann, C. Winnefeld, A. Elham, J. Friedrichs, and R. Hanke-Rauschenbach, Energies 11, 1 (2018). G. Piana, F. Bella, F. Geobaldo, G. Meligrana, and C. Gerbaldi, J. Energy Storage 26, 100947 (2019). S.Toghyani, , F. Baakes, N. Zhang, H. Kühnelt, W. Cistjakov, U. Krewer, J. Electrochem. Soc (2022). Figure 1
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Chometon, Ronan, Marc Dechamps, Jean-Marie Tarascon, and Christel Laberty-Robert. "Meaningful Metrics for an Efficient Solvent-Free Formulation of Polymer – Argyrodite Hybrid Solid Electrolyte." ECS Meeting Abstracts MA2023-02, no. 6 (December 22, 2023): 929. http://dx.doi.org/10.1149/ma2023-026929mtgabs.
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Solid-state batteries generate huge excitement with the promise of higher energy density than current Li-ion technology, thanks to the use of lithium metal at the anode1. Recent advancements in ceramic electrolytes demonstrate comparable conductivity with liquid ones2. However, the brittleness of ceramics results in mechanical limitations, during both assembly and cycling3, constraining the scale-up of pure-ceramic batteries. Hybrid solid electrolytes (HSE) can overcome this hurdle by combining the superior ionic conductivity of inorganic fillers with the scalable process of polymer electrolytes in a unique material. Depending on the amount of ceramic electrolyte, two types of HSE can be prepared: a ceramic-in-polymer approach, in which the inorganic filler disturbs the polymer crystallinity; and a polymer-in-ceramic system where the organic electrolyte mainly acts as a binder. Many parameters such as polymer molar mass, type and concentration of Li salt, chemistry and size of ceramic particles and the mixing route, make the HSE formulation an intricate process. As a result, there is a large disparity in the reported formulations and performances of HSE4. In particular, most approaches focus on a slurry-assisted preparation, which becomes a limiting factor when using sulfide-based electrolytes, as these ceramics degrade in common solvents used for binder processing5. To circumvent these issues, we propose a novel, solvent-free HSE preparation, combining an organic matrix based on poly(ethylene oxide) and lithium bis(trifluoromethanesulfonyl)imide (PEO:LiTFSI), with the highly conductive argyrodite-type Li6PS5Cl. The optimization of the HSE formulation is driven by key metrics, defined as sufficient ionic conductivity (σion ≥ 10-4 S.cm-1 @25°C) and adequate mechanical characteristics (self-standing property and ability to process as thin membrane <100 µm). Through rational screening, we elucidate the impact of formulation parameters and find the organic-to-inorganic ratio, the polymer molar mass and the ratio of mixed polymer lengths to be factors of paramount importance. Our methodology leads to an optimized formulation of the HSE with high ceramic content (75 wt.%) that meets the fixed criteria. Furthermore, we introduce an activation mechanism fitting (Arrhenius or Vulger-Tammann-Fulcher) as a new and effective metric to unravel the ionic pathway within the HSE. A shift in both ionic conductivity, mechanical cohesion and type of activation mechanism is observed at a unique threshold of 75 wt.% ceramic content. We show that our optimized polymer-in-ceramic HSE provides enhanced conduction through the ceramic network (10-4 S.cm-1 @25°C), displaying an Arrhenius activation, compared to ceramic-in-polymer HSEs, which behave as conventional PEO:LiTFSI following a VTF model. This gain in conductivity coincides with a higher mechanical resistance, as confirmed by tensile test on HSE membranes. Probing the compatibility of the organic and inorganic phases, using electrochemical impedance spectroscopy (EIS) alongside solid-state nuclear magnetic resonance (ssNMR), reveals the formation of an interphase, the quantity and resistivity of which grow with time and temperature. Finally, electrochemical performances are evaluated by assembling an HSE-based battery, which displays comparable stability as pure-ceramic ones (> 100 cycles before reaching 20% capacity loss at C/5) but still suffers from higher polarization and thus lower capacity (130 vs 150 mAh.g-1 at C/20). Janek, J. et al., Nat Energy 1, 16141 (2016). Abakumov, A. et al., Nat Commun 11, 4976 (2020). Doux, J.-M. et al., J. Mater. Chem. A 8, 5049–5055 (2020). Horowitz, Y. et al., J. Electrochem. Soc. 167, 160514 (2020). Ruhl, J. et al., Adv. Ener. Sust. Res. 2, 2000077 (2021).
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Song, Shufeng, Masashi Kotobuki, Feng Zheng, Qibin Li, Chaohe Xu, Yu Wang, Wei Dong Z. Li, Ning Hu, and Li Lu. "Al conductive hybrid solid polymer electrolyte." Solid State Ionics 300 (February 2017): 165–68. http://dx.doi.org/10.1016/j.ssi.2016.12.023.
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Bubulinca, Constantin, Natalia E. Kazantseva, Viera Pechancova, Nikhitha Joseph, Haojie Fei, Mariana Venher, Anna Ivanichenko, and Petr Saha. "Development of All-Solid-State Li-Ion Batteries: From Key Technical Areas to Commercial Use." Batteries 9, no. 3 (March 1, 2023): 157. http://dx.doi.org/10.3390/batteries9030157.
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Innovation in the design of Li-ion rechargeable batteries is necessary to overcome safety concerns and meet energy demands. In this regard, a new generation of Li-ion batteries (LIBs) in the form of all-solid-state batteries (ASSBs) has been developed, attracting a great deal of attention for their high-energy density and excellent mechanical-electrochemical stability. This review describes the current state of research and development on ASSB technology. To this end, study of the literature and patents as well as market analysis over the last two decades were carried out, highlighting how scientific achievements have informed the application of commercially profitable ASSBs. Analyzing the patents registered over the past 20 years revealed that the number of them had increased exponentially-from only few per year in early 2000 to more than 342 in 2020. Published literature and patents on the topic declare a solid-state electrolyte (SSE) to be the main component of ASSBs, and most patented examples are referred to as solid inorganic electrolytes (SIEs), followed by solid polymer electrolytes (SPEs) and solid hybrid electrolytes (SHEs) in popularity. Investigation of company websites, social media profiles, reports, and academic publications identified 93 companies associated with ASSBs. A list of leading businesses in the solid-state battery sector was compiled, out of which 36 provided information on the ASSB units in their product portfolio for detailed analysis.
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Zhang, Yinghui, and Jean-François Gohy. "Design of Novel Types of Phosphorus-Containing Flame-Retardant Hybrid Solid Electrolytes with Enhanced Ionic Conductivities." ECS Meeting Abstracts MA2023-02, no. 3 (December 22, 2023): 483. http://dx.doi.org/10.1149/ma2023-023483mtgabs.
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Hybrid polymer/inorganic solid electrolytes have been considered one of the promising routes toward improved safety and higher energy density compared to today’s liquid electrolytes. Herein, flame-retardant phosphorus-containing random copolymers, namely poly(oligo(ethylene glycol) methyl ether methacrylate)-co-(dimethyl(methacryloyloxy)methyl phosphonate) (P(xPEGMA-co-yMAPC1)), were synthesized with different ratio of monomer compositions and further used as the polymer matrix. By mixing P(xPEGMA-co-yMAPC1) with lithium perchlorate (LiClO4) and acetonitrile (ACN), the solid polymer electrolytes were obtained after vacuum evaporation of ACN. Among the P(xPEGMA-co-yMAPC1) copolymer electrolytes, the P(9PEGMA-co-1MAPC1) with 10wt% LiClO4 presented an ionic conductivity of 1.0×10-4 S cm-1 at 60℃ and 3.1×10-5 S cm-1 at 30℃ and showed good flame-retardant performance compared to pure PPEGMA. The increase in MAPC1 content upgraded the flame-retardant performances but enhanced the glass transition temperature (Tg) of the copolymers, leading to a decrease in ionic conductivity. To further enhance the ionic conductivity of the copolymer electrolytes, hybrid polymer/inorganic solid electrolytes are synthesized by adding Li1.3Al0.3Ti1.7(PO4)3 (LATP) and SiO2 inorganic fillers, respectively. P(9PEGMA-co-1MAPC1) with 10wt% LATP exhibits a higher ionic conductivity of 1.4×10-4 S cm-1 at 60℃, while P(9PEGMA-co-1MAPC1) with SiO2 fillers show a lower ionic conductivity of 8.5×10-5 S cm-1 at 60. Finally, the cycling performances of hybrid solid electrolytes containing LiFePO4|P(9PEGMA-co-1MAPC1) + LiClO4 + LATP/SiO2|Li batteries were tested. The capacity reaches 164.2 mAh g−1 at 0.05 C, and the capacity retention reaches 90% after 200 cycles at 0.1 C. Figure 1
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Novakov, Christo, Radostina Kalinova, Svetlana Veleva, Filip Ublekov, Ivaylo Dimitrov, and Antonia Stoyanova. "Flexible Polymer-Ionic Liquid Films for Supercapacitor Applications." Gels 9, no. 4 (April 16, 2023): 338. http://dx.doi.org/10.3390/gels9040338.
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Mechanically and thermally stable novel gel polymer electrolytes (GPEs) have been prepared and applied in supercapacitor cells. Quasi-solid and flexible films were prepared by solution casting technique and formulated by immobilization of ionic liquids (ILs) differing in their aggregate state. A crosslinking agent and a radical initiator were added to further stabilize them. The physicochemical characteristics of the obtained crosslinked films show that the realized cross-linked structure contributes to their improved mechanical and thermal stability, as well as an order of magnitude higher conductivity than that of the non-crosslinked ones. The obtained GPEs were electrochemically tested as separator in symmetric and hybrid supercapacitor cells and showed good and stable performance in the investigated systems. The crosslinked film is suitable for use as both separator and electrolyte and is promising for the development of high-temperature solid-state supercapacitors with improved capacitance characteristics.
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Lim, Seung, Juyoung Moon, Uoon Baek, Jae Lee, Youngjin Chae, and Jung Park. "Shape-Controlled TiO2 Nanomaterials-Based Hybrid Solid-State Electrolytes for Solar Energy Conversion with a Mesoporous Carbon Electrocatalyst." Nanomaterials 11, no. 4 (April 3, 2021): 913. http://dx.doi.org/10.3390/nano11040913.
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One-dimensional (1D) titanium dioxide (TiO2) is prepared by hydrothermal method and incorporated as nanofiller into a hybrid polymer matrix of polyethylene glycol (PEG) and employed as a solid-electrolyte in dye-sensitized solar cells (DSSCs). Mesoporous carbon electrocatalyst with a high surface area is obtained by the carbonization of the PVDC-g-POEM double comb copolymer. The 1D TiO2 nanofiller is found to increase the photoelectrochemical performance. As a result, for the mesoporous carbon-based DSSCs, 1D TiO2 hybrid solid-state electrolyte yielded the highest efficiencies, with 6.1% under 1 sun illumination, in comparison with the efficiencies of 3.9% for quasi solid-state electrolyte and 4.8% for commercial TiO2 hybrid solid-state electrolyte, respectively. The excellent photovoltaic performance is attributed to the improved ion diffusion, scattering effect, effective path for redox couple transfer, and sufficient penetration of 1D TiO2 hybrid solid-state electrolyte into the electrode, which results in improved light-harvesting, enhanced electron transport, decreased charge recombination, and decreased resistance at the electrode/electrolyte interface.
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Foran, Gabrielle, Nina Verdier, David Lepage, Cédric Malveau, Nicolas Dupré, and Mickaël Dollé. "Use of Solid-State NMR Spectroscopy for the Characterization of Molecular Structure and Dynamics in Solid Polymer and Hybrid Electrolytes." Polymers 13, no. 8 (April 8, 2021): 1207. http://dx.doi.org/10.3390/polym13081207.
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Solid-state NMR spectroscopy is an established experimental technique which is used for the characterization of structural and dynamic properties of materials in their native state. Many types of solid-state NMR experiments have been used to characterize both lithium-based and sodium-based solid polymer and polymer–ceramic hybrid electrolyte materials. This review describes several solid-state NMR experiments that are commonly employed in the analysis of these systems: pulse field gradient NMR, electrophoretic NMR, variable temperature T1 relaxation, T2 relaxation and linewidth analysis, exchange spectroscopy, cross polarization, Rotational Echo Double Resonance, and isotope enrichment. In this review, each technique is introduced with a short description of the pulse sequence, and examples of experiments that have been performed in real solid-state polymer and/or hybrid electrolyte systems are provided. The results and conclusions of these experiments are discussed to inform readers of the strengths and weaknesses of each technique when applied to polymer and hybrid electrolyte systems. It is anticipated that this review may be used to aid in the selection of solid-state NMR experiments for the analysis of these systems.
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Popovic-Neuber, Jelena. "Interfacial Chemistry and Electrolyte Approaches for Enabling Metal Anode Batteries." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 205. http://dx.doi.org/10.1149/ma2022-023205mtgabs.
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Continuous solid electrolyte interphase (SEI) and dendrite growth, as well as formation of ion blocking interfaces are some of the crucial issues preventing the commercialization of batteries depending on the implementation of Li/Na/K/Mg/Ca metal anodes.[1,2] In the first part of my talk, I will focus on the chemistry of formed interfaces, including growth and ion transport control. Second part of my talk deals with bulk liquid, polymer and hybrid electrolyte molecular structure approaches for circumventing dendrite formation. Understanding of the SEI growth on alkali and alkaline earth metals in contact with liquid electrolytes under open circuit potential conditions important for shelf aging is still in its infancy. I will show that the SEI formed on Li in contact with glyme-based electrolyte grows via reaction-controlled mechanism that is rapidly substituted by the diffusion-controlled one.[3] The ionic transport and stability of the complex composite SEI material under current is highly dependent on the salt chemistry, with detrimental effects of LixSy and positive effects of the Li3N constituents. Most recent ion transport and morphological studies show that the initial SEI formed in contact with liquid electrolytes on Li, Na and Mg is nanoporous.[4,5] Based on the electrochemical impedance spectroscopy measurements in symmetric cells and related equivalent circuit models, I will discuss potential growth mechanism via SEI densification. Finally, I will present a possibility of using gas/solid synthesis for preparation of sulfide-based artificial SEIs for both liquid-based and solid-state batteries.[6] Dendrite formation on alkali and alkaline earth metal anodes is closely related to the ion concentration gradients formed near the electrodes in contact with the electrolytes. I will discuss the method to circumvent this problem by using electrolytes with high cationic transference number. In soft matter electrolytes this is possible when (i) interfacial effect enables preferential anionic adsorption in liquid/solid electrolytes,[7] (ii) the size and steric effects control the association and mobility of the anion in the liquid electrolytes,[8] (iii) ion transport proceeds through percolating amorphous clusters in polymer-in-salt electrolytes. [9] References: [1] J. Popovic, Nat. Comm., 12, 6240 (2021) [2] J. Popovic, J. Electrochem. Soc., 3, 169 030510 (2022) [3] M. Nojabaee, K. Küster, U. Starke, J. Popovic, J. Maier, Small, 16, 23, 2000756 (2020) [4] K. Lim, B. Fenk, J. Popovic, J. Maier, ACS App. Mat. Int., 13 (43), 51767 (2021) [5] J. Popovic, Energy Technol., 9, 4, 2001056 (2021) [6] K. Lim, B. Fenk, K. Küster, T. Acartürk, J. Weis, U. Starke, J. Popovic, J. Maier, ACS App. Mat. Int., 10.1021/acsami.1c23923 (2022) [7] J. Popovic, G. Hasegawa, I. Moudrakovski, J. Maier, J. Mat. Chem. A, 1, 40, 7135 (2016) [8] J. Popovic, D. Höfler, J. Melchior, A. Münchinger, B. List, J. Maier, J. Phys. Chem. Lett., 9, 17, 5116 (2018) [9] J. Popovic, Macromol. Chem. Phys, 10.1002/macp.202100344 (2021)
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Bristi, Afshana Afroj, Alfred Samson, and Venkataraman Thangadurai. "Na Plating and Stripping Using Highly Na-Ion Conductive Solid Polymer Electrolytes Based on Polyvinylidene Fluoride and Polyvinylpyrrolidone." ECS Meeting Abstracts MA2022-01, no. 4 (July 7, 2022): 536. http://dx.doi.org/10.1149/ma2022-014536mtgabs.
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Solid-state sodium-ion batteries (ss-SIBs) are a promising alternative to commercially available lithium-ion batteries (LIBs) for next-generation energy storage applications. They have lower production costs and are safer than LIBs. Moreover, sodium is more abundant than lithium. The incorporation of solid polymer electrolytes (SPEs) into SIBs has been attracting much more attention due to the easy processability, low costs, safe usability, modification scope, and abundance of polymers. However, SPEs for ss-SIBs with high ionic conductivity and low interfacial resistance between electrolytes and electrodes are lacking. In addition, SPEs face major challenges such as suitable manufacturing methods and the lack of knowledge about low-cost ss-SIBs assembly. Herein, using a facile solution casting process, we have successfully fabricated a high sodium-ion conductive composite SPE film based on polyvinylidene fluoride (PVDF) polymer, polyvinylpyrrolidone (PVP) binder, and NaPF6 salt. A comprehensive characterization has been conducted using X-Ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Fourier Transform Infrared (FTIR), Thermogravimetric Analysis (TGA), Raman, and electrochemical impedance spectroscopy techniques to investigate the structural, thermal, and electrochemical performance of the as-prepared SPE films. High ionic conductivity (8.51 x 10-4 S cm-1 and 8.36 x 10-3 S cm-1 at 23°C and 78 °C, respectively) was observed from the SPE. A hybrid symmetric half-cell assembly (Na foil + 20 µL of 1 M NaClO4 in ethylene carbonate (EC) and propylene carbonate (PC) (EC: PC = 1:1) + Carbon-cloth |SPE| Carbon-cloth + 20 µL of 1 M NaClO4 in EC and PC (EC: PC = 1:1) | Na foil) showed excellent Na plating-stripping performance up to 8 mA cm-2 for 100 cycles. In addition, Na+ transfer mechanism in the composite electrolyte has been investigated using impedance and dielectric spectroscopy. The results indicate the promising applicability of SPEs in next-generation high-power rechargeable SIBs.
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Lee, Sukhyung, Junsik Kang, and Hochun Lee. "Dual Electrolyte Additives Enabling Bilayer SEI to Suppress Hydrogen Evolution Reaction in Aqueous Li-Ion Batteries." ECS Meeting Abstracts MA2023-01, no. 2 (August 28, 2023): 545. http://dx.doi.org/10.1149/ma2023-012545mtgabs.
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Aqueous Li-ion batteries (LIBs) feature safe operation, low cost, and environmental friendliness, but suffer from low energy density due to narrow electrochemical stability window (ESW) of aqueous electrolytes. While exploiting high-salt-concentration strategy of water-in-salt electrolytes (WiSEs) is effective in improving the electrochemical stability, the improvement is still insufficient to ensure practical feasibility of aqueous LIBs. In particular, the reduction stability of WiSEs needs further improvement to enable stable operation of low-voltage anode materials including Li4Ti5O12. This talk reports that the co-use of two electrolyte additives can effectively expand the cathodic limit of various WiSE systems. The synergistic effect between the two additives is attributed to the formation of unique solid-electrolyte interphase composed of organic and inorganic bilayers. The inner inorganic layer suppresses hydrogen evolution reaction, while the outer hydrophobic organic polymer mitigates the dissolution of inner SEI. LiMn2O4/Li4Ti5O12 cells employing 21 m LiTFSI WISE with the dual additives exhibit excellent long-term cycling (>70% retention after 400 cycles at 25 oC) and good rate capability (110 mAh/g at 6 mA/cm2). The efficacy of the dual-additive approach is also demonstrated for other WiSE solutions including water-in-bisalt, hydrate melt, and aqueous/organic hybrid electrolytes, suggesting the general applicability of the dual-additive strategy. Figure 1
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Yang, Guang, Yaduo Song, and Longjiang Deng. "Polyaddition enabled functional polymer/inorganic hybrid electrolytes for lithium metal batteries." Journal of Materials Chemistry A 9, no. 11 (2021): 6881–89. http://dx.doi.org/10.1039/d0ta11730g.
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Pang, Quan, Laidong Zhou, and Linda F. Nazar. "Elastic and Li-ion–percolating hybrid membrane stabilizes Li metal plating." Proceedings of the National Academy of Sciences 115, no. 49 (November 19, 2018): 12389–94. http://dx.doi.org/10.1073/pnas.1809187115.
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Lithium metal batteries are capable of revolutionizing the battery marketplace for electrical vehicles, owing to the high capacity and low voltage offered by Li metal. Current exploitation of Li metal electrodes, however, is plagued by their exhaustive parasitic reactions with liquid electrolytes and dendritic growth, which pose concerns to both cell performance and safety. We demonstrate that a hybrid membrane, both elastic and Li+-ion percolating, can stabilize Li plating/stripping with high Coulombic efficiency. The compact packing of a Li+ solid electrolyte phase offers percolated Li+-conducting channels and the consequent infiltration of an elastic polymer endows membrane flexibility to accommodate volume changes. The protected electrode allows Li plating with 95.8% efficiency for 200 cycles and stable operation of an LTO|Li cell for 2,000 cycles. This rationally structured membrane represents an interface engineering approach toward stabilized Li metal electrodes.
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Munichandraiah, N., G. Sivasankar, L. G. Scanlon, and R. A. Marsh. "Characterization of PEO-PAN hybrid solid polymer electrolytes." Journal of Applied Polymer Science 65, no. 11 (September 12, 1997): 2191–99. http://dx.doi.org/10.1002/(sici)1097-4628(19970912)65:11<2191::aid-app16>3.0.co;2-6.
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Hatakeyama-Sato, Kan, Yasuei Uchima, Takahiro Kashikawa, Koichi Kimura, and Kenichi Oyaizu. "Extracting higher-conductivity designs for solid polymer electrolytes by quantum-inspired annealing." RSC Advances 13, no. 21 (2023): 14651–59. http://dx.doi.org/10.1039/d3ra01982a.
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Allam, Omar, and Seung Soon Jang. "Multiscale Simulation of Carbonate-Based Electrolytes for Li-Ion Battery." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 311. http://dx.doi.org/10.1149/ma2022-023311mtgabs.
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Organic electrodes have been extensively studied for their application as cathode materials for Li-ion battery due to their relatively inexpensive synthesis, earth-abundant precursors, and their high-rate capabilities. In our previous studies, we developed hybrid machine learning-density functional theory protocols to predict and analyze the redox potentials for novel organic moieties. Although the prediction of the electrochemical activity is critical for the design of high energy density cathodes, one of the most detrimental challenges facing the practical application of organic electrode materials is their dissolution by liquid electrolytes. Therefore, it is necessary to investigate several avenues to curb this undesirable dissolution by the electrolyte. In this fundamental study, we investigate novel carbonate-based solid-polymer electrolytes (SPE) using MD simulations and compare their performance to their conventional liquid carbonate electrolyte counterparts. Specifically, we characterize how the nanophase morphology of the amorphous polycarbonate systems is affected by modulating the composition of the carbonate side chains, while comparing them with their liquid electrolyte counterparts such as dimethyl carbonate and ethylene carbonate. Moreover, our study will elucidate how the morphology and thermodynamic properties, such as glass transition temperature, are affected by using aliphatic vs aromatic carbonate side chains, mixing of the side chain types, as well as by adjusting the length of the spacer carbon chain between the carbonate groups and the main chain. Therefore, this investigation can provide valuable insight regarding the optimal polymeric composition and mixture to achieve a morphology that is desirable for enhanced ion transport, while also inhibiting the disintegration of the organic cathode by the electrolyte.
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Lashkari, Sima, Daniela de Morais Zanata, Nicolas Goujon, Ousmane Camara, David Mecerreyes, and Irune Villaluenga. "Solid-State Redox-Active Pseudocapacitor with Improved Performance at High Temperature." ECS Meeting Abstracts MA2023-02, no. 1 (December 22, 2023): 6. http://dx.doi.org/10.1149/ma2023-0216mtgabs.
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With the emergence of environmental issues such as global warming as well as our new demand for efficient energy storage systems (EES) that can power portable electronics; batteries and supercapacitors are gaining more attention in the latest literature. Batteries can provide high energy density and lower power densities (e.g. for LIB, 1kW.kg-1 vs. 150-200 Wh.kg-1), while supercapacitors are high power devices with low energy densities (e.g. for most commercial devices ⁓ 10 kW.kg-1 vs. 5-10 Wh.kg-1). In order to couple high energy and high power densities of both devices, pseudocapacitance was introduced in 1991 by Conway 1 using metal oxide. Pseudocapacitance is a fast and reversible surface faradaic process with performance similar to double layer capacitors but higher energy densities closer to that of batteries. Aside from metal oxides, conductive polymers also demonstrate pseudocapacitance. In this regards, the use of conductive polymers as nontoxic, abundant, low cost and sustainable organic material is on the rise. Nevertheless, the inherent issue related to instability of the conductive polymer especially at high degree of oxidation had restricted their application in EES. However, redox active polymers (RAPs) with non-conjugated backbone and redox active pendant group demonstrates improved performance and structural diversity with more distinct redox potentials. 2 Amongst them, quinone-containing polymers with their high theoretical capacities, facile kinetics and tunable redox potential are at the top of the list. Particularly, catechol, a bioinspired ortho-quinone based polymer has gain popularity following a work by Detrembleur et al. 3 However; the solubility of the organic materials in organic solvents hinders their application in EES. To this end, using solid-state electrolyte can help alleviate the issue. Nevertheless, solid-state design stimulate sluggish kinetics and reduce electrode/electrolyte interfacial area, a component required to achieve high pseudocapacitance. Consequently, nano-structuring the redox polymer can help improve the contact resistance as well as increasing the surface area. In addition, the nanoparticles structure will promote more distinct redox processes. 4 In this study, we demonstrate for the first time, a prototype pouch cell based on all-solid-state organic hybrid supercapacitor bearing catechol redox active moieties. Using emulsion polymerization, catechol based RAP nanoparticles of size ranging from 50 to 150 nm were synthesized 4 and together with activated carbon was used as working electrode. Block-co-polymers based solid electrolyte was employed as electrolyte as well as binder for both cathode and anode. Using this design, discharge capacities of ⁓ 10 and 60 mAh/g at room temperature and at 50 °C were obtained, respectively. References: (1) Conway, B. E. Transition from “Supercapacitor” to “Battery” Behavior in Electrochemical Energy Storage. J. Electrochem. Soc. 1991, 138 (6), 1539. https://doi.org/10.1149/1.2085829. (2) Casado, N.; Mecerreyes, D. Redox Polymers for Energy and Nanomedicine; Royal Society of Chemistry, 2020. (3) Patil, N.; Aqil, M.; Aqil, A.; Ouhib, F.; Marcilla, R.; Minoia, A.; Lazzaroni, R.; Jérôme, C.; Detrembleur, C. Integration of Redox-Active Catechol Pendants into Poly(Ionic Liquid) for the Design of High-Performance Lithium-Ion Battery Cathodes. Chem. Mater. 2018, 30 (17), 5831–5835. https://doi.org/10.1021/acs.chemmater.8b02307. (4) Gallastegui, A.; Camara, O.; Minudri, D.; Goujon, N.; Patil, N.; Ruipérez, F.; Marcilla, R.; Mecerreyes, D. Aging Effect of Catechol Redox Polymer Nanoparticles for Hybrid Supercapacitors. Batter. Supercaps 2022, 5 (9), e202200155. https://doi.org/10.1002/batt.202200155.
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Luo, Wen-Bin, Shu-Lei Chou, Jia-Zhao Wang, Yong-Mook Kang, Yu-Chun Zhai, and Hua-Kun Liu. "A hybrid gel–solid-state polymer electrolyte for long-life lithium oxygen batteries." Chemical Communications 51, no. 39 (2015): 8269–72. http://dx.doi.org/10.1039/c5cc01857a.
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A gel–solid state polymer electrolyte has been used as the separator and an electrolyte for lithium oxygen batteries, which can not only avoid electrolyte evaporation but also protect the lithium metal anode during reactions over long-term cycling.
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Chelfouh, Nora, Steeve Rousselot, Gaël Coquil, Gabrielle Foran, Lea Caradant, Fatemeh Shoghi, Elsa Briqueleur, Audrey Laventure, and Mickael Dolle. "Using Pectin for Energy Storage Devices." ECS Meeting Abstracts MA2023-01, no. 5 (August 28, 2023): 891. http://dx.doi.org/10.1149/ma2023-015891mtgabs.
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Wearable and flexible printed electronics are more than ever in demand. The value of the flexible electronics market reached USD 26.5 million in 2021 and its revenue forecast will reach USD 63.1 million in 2030.[1] Increasing investments in research & development in these fields have already led to several achievements in the past years. Nevertheless, serious remains concerns about the ecological footprint of such technologies must be addressed early in their conception and throughout the whole electronics life cycle.[2] In printed electronics, electrical energy is supplied by energy storage devices, such as batteries. Most of the time, these systems contain polymers that can be used either as electrolyte, e.g., solid polymer electrolyte or gel polymer electrolyte, to facilitate flexible electronics/batteries fabrication or as binders in positive or negative electrodes ensuring the mechanical cohesion within the composite electrodes.[4]. Several characteristics to meet environmental-friendly flexible electronics requirements. Biobased polymers are one of the promising alternatives in this regard. Their general affinity with water makes them suitable for aqueous rechargeable batteries, implying several technologies such as aqueous rechargeable lithium-ion batteries (ARLB) or zinc rechargeable batteries (ZRB). For instance, polymer hydrogel electrolytes have recently been investigated [3]: their strength lies in promising ionic conductivity (> 10-2 S.cm-1) while maintaining a sufficient mechanical strength and elasticity to be adaptable to flexible energy storage devices. In this study, we developed a hydrogel electrolyte made of pectin, a polysaccharide contained in the cell plants’ wall, as an alternative to synthetic polymers in batteries. Hydrophobic interactions and hydrogen bonds, together with bivalent cation interactions, allow the free-standing electrolyte gelation.[5] The gelation mechanism is first studied, using NMR spectroscopy together with thermal analysis. Then, electrochemical characterization is carried out to analyze the ionic conduction pathways of the gel electrolyte. Its electrochemical stability as well as galvanostatic cycling are investigated to figure out its ability to be used as a electrolyte in hybrid device, such as zinc-lithium-ion batteries. Moving toward printed devices requires to take a closer look to the rheological properties of this system as well as its printability: these challenges will be addressed to ultimately develop an understanding of the impact of this material’s processing on the electrolyte and electrodes properties.[6] References [1]. Flexible Electronics Market Size to Hit US$ 63.1 MN by 2030. (May 2022). Acumen Research and Consulting, https://www.acumenresearchandconsulting.com/. [2]. Baran, D.; Corzo, D.; Blazquez, G. Flexible Electronics: Status, Challenges and Opportunities. Frontiers in Electronics 2020, 1, 2673-5857. DOI: 10.3389/felec.2020.594003. [3]. Liu, J.; Yuan, H.; Tao, X.; et al. Recent progress on biomass-derived ecomaterials toward advanced rechargeable lithium batteries. EcoMat 2020, 2 (1), e12019. DOI: 10.1002/eom2.12019. [4]. Bresser, D.; Buchholz, D.; Moretti, A.; Varzi, A.; Passerini, S. Alternative binders for sustainable electrochemical energy storage – the transition to aqueous electrode processing and bio-derived polymers. Energy Environm Sci 2018, 11, 3096-3127. DOI: 10.1039/C8EE00640G. [5]. Chelfouh, N.; Coquil, G.; Rousselot, S.; Foran, G.; Briqueleur, E.; Shoghi, F.; Caradant, L.; Dollé, M. Apple Pectin-Based Hydrogel Electrolyte for Energy Storage Applications. ACS Sustainable Chemistry & Engineering 2022 , Article ASAP . DOI: 10.1021/acssuschemeng.2c04600. [6]. Clement, B.; Lyu, M.; Kulkarni, S. E.; Lin, T.; Hu, Y.; Lockett, V.; Greig, C.; Wang, L. Recent Advances in Printed Thin-Film Batteries. Engineering 2022, 13, 238-261. DOI: 10.1016/j.eng.2022.04.002.
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Hao, Shuai, Lei Li, Wendong Cheng, Qiwen Ran, Yuyao Ji, Yuxuan Wu, Jinsheng Huo, Yingchun Yang, and Xingquan Liu. "Long-chain fluorocarbon-driven hybrid solid polymer electrolyte for lithium metal batteries." Journal of Materials Chemistry A 10, no. 9 (2022): 4881–88. http://dx.doi.org/10.1039/d1ta10728c.
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Scheller, Maximilian, Axel Durdel, Johannes Kriegler, Alexander Frank, and Andreas Jossen. "Simulation of Hybrid All-Solid-State Battery Performance Under Consideration of Ceramic-Polymer Phase Boundaries Using a Physicochemical Modelling Approach." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 992. http://dx.doi.org/10.1149/ma2023-016992mtgabs.
Full textAbstract:
With the growing interest in all-solid-state battery (ASSB) technology for high-energy and high-power applications, the electrochemical performance of cell components and production-related characteristics must be improved to achieve reliable and cost-effective scale-up of laboratory cell concepts [1]. Combining inorganic ceramic and polymer solid electrolytes (SEs) serves to tune the ionic transport and the mechanical properties of composite cathodes [2, 3]. A polymer electrolyte share in the composite cathode is expected to improve the mechanical contact between the cathode active material (CAM) and the SE, resulting in facilitated charge transfer and improved cell performance. Furthermore, polymer SEs serve to overcome the challenges of co-sintering dense composites of CAM and inorganic SE [4, 5]. In hybrid cell concepts with polymer- and inorganic ceramic SE, the ionic transport path crosses a ceramic-polymer phase boundary, which leads to additional polarization through charge transfer and ohmic resistance. State-of-the-art literature discusses the influence of ceramic particles in polymer electrolytes, but falls short on the impact of ceramic-polymer phase boundaries on the total cell performance of ASSBs [6, 7, 8]. To allow for the simulation of hybrid full cells, a pseudo-two-dimensional (p2D) physicochemical model is introduced within this work. The model is based on the Newman approach, modified with a description for the ceramic-polymer phase boundary [9]. In equilibrium state, the potential drop across the ceramic-polymer boundary was modeled with the Donnan-potential condition as recently proposed by Kim et al. [10]. Under current flow, additional polarization occurs at the interface due to electrochemical charge transfer, which was modeled by the Butler-Volmer equation, and ohmic contact resistance. The conservation of mass and charge over the phase boundary was secured with a current, flux, and a potential boundary condition. A model cell was defined (see figure 1) and parametrized using material-specific values for the ionic and electronic transport characteristics as well as the interface and charge transfer properties. Since the focus of this study was on the ceramic-polymer phase boundary, ideal plating and stripping behavior at the Li-metal anode were assumed neglecting irregular lithium deposition, e.g., lithium dendrite formation. As separator material, the well-known ceramic LLZO SE was modeled. A composite cathode with NMC-622 as CAM and PEO/LiTFSI as polymer electrolyte was assumed. The lower part of figure 1 shows the reduced 1D-model geometry and the ion transport mechanisms in each model domain. The established physicochemical model was applied to identify performance-limiting effects in hybrid ASSBs to conclude on cell designs achieving high energy and power densities. To quantify and localize the polarization contributions in each domain, arising from SE ionic conductivity, diffusion or charge-transfer processes, as well as phase boundaries, the method proposed by Nyman et al. was used [11]. Figure 2 a) shows the results of polarization analysis when simulating a 0.1C charge, while figure 2 b) depicts the results for a 1C charge. Diffusion limitation in the polymer electrolyte led to high concentration gradients in the polymer-phase of the composite cathode, resulting in high diffusion polarization at elevated charging rates as shown in figure 2 b). This determined a critical current density at cell level, which was caused by large Li-ion concentration gradients and a possible depletion of Li-ions near the ceramic separator. The overall cell polarization was further enhanced by the ceramic-polymer phase boundary. For the contact case of LLZO versus PEO/LiTFSI considered here, the equilibrium potential between the phases was calculated according to the theory of Donnan to 31 mV. Since a wide range of values for the contact resistance at the ceramic-polymer interface is reported in the literature [6, 7], ohmic polarization could be important and was therefore evaluated as a function of different contact resistances. A critical contact resistance was determined to achieve the requirements for future battery technologies regarding energy and power density. Figure 1