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Kanai, Yamato, Koji Hiraoka, Mutsuhiro Matsuyama i Shiro Seki. "Chemically and Physically Cross-Linked Inorganic–Polymer Hybrid Solvent-Free Electrolytes". Batteries 9, nr 10 (26.09.2023): 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 i Pilwon Heo. "(Invited) Pragmatic Approach and Challenges of All Solid State Batteries: Hybrid Solid Electrolyte for Technical Innovation". ECS Meeting Abstracts MA2023-01, nr 6 (28.08.2023): 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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LI, X. D., X. J. YIN, C. F. LIN, D. W. ZHANG, Z. A. WANG, Z. SUN i 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, nr 04 (sierpień 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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Lv, Wenjing, Kaidong Zhan, Xuecheng Ren, Lu Chen i Fan Wu. "Comparing Charge Dynamics in Organo-Inorganic Halide Perovskite: Solid-State versus Solid-Liquid Junctions". Journal of Nanoelectronics and Optoelectronics 19, nr 2 (1.02.2024): 121–28. http://dx.doi.org/10.1166/jno.2024.3556.
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In this study, we explore the dynamics of a perovskite-electrolyte photoelectrochemical cell, pivotal for advancing electrolyte-gated field effect transistors, water-splitting photoelectrochemical and photocatalytic cells, supercapacitors, and CO2 capture and reduction technologies. The instability of hybrid perovskite materials in aqueous electrolytes presents a significant challenge, yet recent breakthroughs have been achieved in stabilizing organo-inorganic halide perovskite films. This stabilization is facilitated by employing liquid electrolytes, specifically those formed by dissolving tetrabutylammoniumperchlorate in dichloromethane. A critical aspect of this research is the comparative analysis of charge and ion kinetics at the perovskite/liquid electrolyte interface versus the perovskite/solid charge transport layer interface. Employing Intensity Modulated Photocurrent Spectroscopy (IMPS), Open-Circuit Voltage Decay (OCVD), and Capacitance-Frequency (C-F) methods, the study scrutinizes charge dynamics in both perovskite/electrolyte and perovskite/solid interfaces. Furthermore, the investigation extends to contrasting the properties of solid–liquid and solid-state junctions, focusing on mobile ions, electric field impacts, and electron-hole transport. The research also examines variations in recombination resistance and ionic double layer charging in perovskite-based devices, aiming to elucidate the operational mechanisms and kinetic complexities at the hybrid perovskite/electrolyte interface.
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Liao, Cheng Hung, Chia-Chin Chen, Ru-Jong Jeng i 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, nr 6 (28.08.2023): 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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Villaluenga, Irune, Kevin H. Wujcik, Wei Tong, Didier Devaux, Dominica H. C. Wong, Joseph M. DeSimone i Nitash P. Balsara. "Compliant glass–polymer hybrid single ion-conducting electrolytes for lithium batteries". Proceedings of the National Academy of Sciences 113, nr 1 (22.12.2015): 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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Zaman, Wahid, Nicholas Hortance, Marm B. Dixit, Vincent De Andrade i Kelsey B. Hatzell. "Visualizing percolation and ion transport in hybrid solid electrolytes for Li–metal batteries". Journal of Materials Chemistry A 7, nr 41 (2019): 23914–21. http://dx.doi.org/10.1039/c9ta05118j.
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Zahiri, Beniamin, Chadd Kiggins, Dijo Damien, Michael Caple, Arghya Patra, Carlos Juarez Yescaz, John B. Cook i Paul V. Braun. "Hybrid Halide Solid Electrolytes and Bottom-up Cell Assembly Enable High Voltage Solid-State Lithium Batteries". ECS Meeting Abstracts MA2022-01, nr 2 (7.07.2022): 327. http://dx.doi.org/10.1149/ma2022-012327mtgabs.
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Interface between halide based solid electrolytes and layered transition metal oxide cathodes has been found to be electro-chemically stable due to stability of chloride compounds, in particular, at >4V range. The extent of interfacial stability is correlated with the type of cationic and anionic species in the solid electrolyte compound, a fact supported by theoretical prediction and yet, not accurately measured in composite cathode mixtures. By altering the architecture of cathode into a dense additive-free structure, we have identified differences in interfacial stability of chloride compounds which are hidden in composite cathode formats. In this work, we report the use of dense cathode to track the electrochemical evolution of interface between a hybrid halide solid electrolyte composed of chloride and fluoride species. Introducing fluoride compounds is known to be a promising method to expand the oxidation stability while the nature of such expansion is found to be related to kinetics rather than thermodynamics, we report. Furthermore, fluorination of solid electrolyte is generally accompanied with loss of ionic conductivity due to strong electronegative fluoride ions. We demonstrate a fundamental change of solid-state battery assembly from conventional electrolyte pelletizing followed by electrode placement, to a bottom-up assembly route starting with dense cathode, thin (<20µm) layer of SE and anode addition, which compensates for the suppressed conductivity of fluorinated halide solid electrolytes. Through extensive characterization, compositional optimization, and electrochemical interfacial analysis, we demonstrate stable cycling of LiCoO2/hybrid halide solid electrolyte up to 4.4V vs. Li. Our findings pave the way for expanding the voltage stability of solid electrolytes without compromising the cell performance due to ionic conductivity overpotential issues.
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Mohanty, Debabrata, Shu-Yu Chen i 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, nr 10 (9.10.2022): 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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Gu, Sui, Xiao Huang, Qing Wang, Jun Jin, Qingsong Wang, Zhaoyin Wen i Rong Qian. "A hybrid electrolyte for long-life semi-solid-state lithium sulfur batteries". Journal of Materials Chemistry A 5, nr 27 (2017): 13971–75. http://dx.doi.org/10.1039/c7ta04017b.
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Woolley, Henry Michael, i Nella Vargas-Barbosa. "Electrochemical Characterization of Thiophosphate- Ionic Liquid Hybrid Lithium Electrolytes Against Li Metal". ECS Meeting Abstracts MA2023-01, nr 6 (28.08.2023): 986. http://dx.doi.org/10.1149/ma2023-016986mtgabs.
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(Almost) solid-state batteries that utilize thiophosphate solid electrolytes (SE) are an exciting technology emerging as a potential alternative to lithium-ion batteries. When used alongside a lithium metal anode they can offer the high energy densities [1] required to meet the increasing demand for energy storage. However, they suffer from numerous issues which predominately occur at the cathode- or anode-SE interface. Issues include dendrite propagation through gaps, pores and grain boundaries of the solid electrolyte which can eventually puncture electrolyte crystallites and lead to cell failure. [2] Thiophosphate electrolytes are also unstable both chemically and electrochemically. As a result of the SEs having a low electrochemical stability window reduction or oxidation can occur at the anode or cathode interface, forming a resistive solid electrolyte interphase (SEI). [3] Finally, the ionic contact between Li metal anode and electrolyte is poor and thus high interfacial impedances can arise. These impedances can be dynamic which increase during stripping of the lithium and decrease during plating. [4] To solve some of the interfacial issues there is the option to add a small of amount of liquid electrolyte at the lithium metal-electrolyte interface. The liquid electrolyte can fill in the gaps and pores at the interface thus improving the ionic contact whilst allowing a more stable interface. Whilst the ionic contact can be improved the inherent instability of thiophosphate electrolytes against the liquid electrolyte means that a new interphase known as the solid-liquid electrolyte interphase (SLEI) can form. The presence of this interphase can therefore lower the energy density and round-trip efficiencies of cells which utilize hybrid electrolytes meaning that minimizing the SLEI resistance and maximizing total ionic conductivities is important in hybrid cells. [5] In this work a hybrid of the thiophosphate argyrodite Li6PS5Cl and the ionic liquid x-LiTFSI-1-butyl 1-methylpiperidinium TFSI (BMPipTFSI) with LiTFSI concentrations of 0.25 M and 0.5 M was studied. The choice of SE and liquid electrolyte boils down to the high ionic conductivity of the SE and the electrochemical and thermal stability of the ionic liquid. Temperature-dependent ionic conductivity measurements showed that hybrid systems exhibit lower in room temperature ionic conductivities and higher total activation energies. This hints at the presence of a SLEI forming between the LE and SE. To study how the SLEI resistances changes over time, ion blocking potential impedance spectroscopy measurements were performed. These measurements were performed at 10 °C to allow for the resistance contributions to be better resolved and showed a SLEI resistance of around 45-50 Ω cm2 for both hybrids. Over the period of 130 hours this resistance changed minimally (around 5 Ω cm2 on average) indicating good stability of the SLEI. To further test the suitability of this hybrid alongside lithium metal anodes impedance measurements in symmetrical lithium cells (Li0|LE|LPCL|LE|Li0) were undertaken. In this case galvanostatic impedance spectroscopy (GEIS) with an applied current density of ±0.4 mA cm-2 was used to probe the changes in resistance contributions in the system over the period of stripping (positive current) and plating (negative current). For cells with just SE a large change in the resistance owing to the electrochemical reaction (ECR) (Li0 ↔ Li+ + e-) occurred during stripping and plating indicating the dynamic nature of the ionic contact at the interface. For the hybrid electrolyte cells, this ECR resistance is decreased and becomes more stable however a larger interphase resistance is present. This resistance is a combination of the resistances of both the SLEI (the interphase between the LE and SE) and the SEI (the interphase between LE and Li anode) and it changes over stripping and plating showing that the S(L)EIs which are present are dynamic. Finally, post-mortem SEM/EDX of the surface of samples show a change in morphology and the presence of decomposition products from both the liquid and solid electrolytes. These studies show that the LPCL-BMPipTFSI hybrid is stable and improve ionic contact at the lithium metal anode interface. Further testing in half Li-S cells will determine the suitability of the use of the ionic liquid at the cathode side of the cell. References [1] J. Janek and W. G. Zeier, Nat Energy, 2016, 1, 16141. [2] M. B. Dixit et al. Matter, 2020, 3, 2138-2159 [3] G. Dewald et al. Chem Mater, 2019, 31, 8328-8337. [4] T. Krauskopf et al. Chem. Rev, 2020, 7745-7794. [5] H. M. Woolley and N. M. Vargas-Barbosa, under review.
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CHENG, Xiong, Man LI, Yang Li, Seunghyun Song, Sowjanya Vallem i Joonho Bae. "Novel DNA-Based Polymer Solid Electrolytes for Lithium-Ion Batteries". ECS Meeting Abstracts MA2024-01, nr 2 (9.08.2024): 350. http://dx.doi.org/10.1149/ma2024-012350mtgabs.
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Solid electrolytes are becoming increasingly popular due to their safety [1], and the application of organic biomolecules in electrochemical devices is also an important strategy for sustainable development [2]. Recently, we have studied the application of DNA in electrochemical energy storage devices [3]. A novel PVDF@DNA solid polymer electrolyte was designed in this work, we studied the effect of different DNA addition amounts on polymer solid electrolytes. DNA as a plasticizer-like additive, reduces the crystallinity of the polymer solid electrolyte and improves its ionic conductivity [4]. At the same time, due to the Lewis acid effect of DNA, it can promote the dissociation of lithium salt when interacting with lithium salt anions, and it can also fix the anions, causing more free lithium ions in the electrolyte, thus improving its ionic conductivity. The polymer solid electrolyte with DNA shows relatively better performance. Hence, the DNA-based polymer solid electrolyte fabricated in this study has substantial potential for application in LSBs. Acknowledgement This work was supported by the National Research Foundation of Korea (NRF-2021R1A2C1008272). This work was supported by Ministry of Trade, Industry and Energy, KEIT, under the project title "International standard development of evaluation methods for nano-carbon-based high-performance supercapacitors for electric vehicles" (project # 20016144). References [1] Liang J. et al. Recent progress on solid-state hybrid electrolytes for solid-state lithium batteries. Energy Storage Materials 21 (2019) 308-334. [2] Dutta, D. et al. N7-(carboxymethyl)guanine-Lithium Crystalline Complex: A Bioinspired Solid Electrolyte. Scientific Reports 6 (2016) 24499. [3] Xue Y. et al. DNA-directed fabrication of NiCo2O4 nanoparticles on carbon nanotubes as electrodes for high-performance battery-like electrochemical capacitive energy storage device. Nano Energy 56 (2019) 751–758. [4] Li Z. et al. Ionic Conduction in Polymer-Based Solid Electrolytes. Advanced Science 10 (2023) 2201718.
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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 i in. "Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries". Inorganics 10, nr 5 (26.04.2022): 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 i in. "Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries". Inorganics 10, nr 5 (26.04.2022): 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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Vargas-Barbosa, Nella Marie, Sebastian Puls i Henry Michael Woolley. "Hybrid Material Concepts for Thiophosphate-Based Solid-State Batteries". ECS Meeting Abstracts MA2023-01, nr 6 (28.08.2023): 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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Shah, Rajesh, Vikram Mittal i Angelina Mae Precilla. "Challenges and Advancements in All-Solid-State Battery Technology for Electric Vehicles". J 7, nr 3 (27.06.2024): 204–17. http://dx.doi.org/10.3390/j7030012.
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Recent advances in all-solid-state battery (ASSB) research have significantly addressed key obstacles hindering their widespread adoption in electric vehicles (EVs). This review highlights major innovations, including ultrathin electrolyte membranes, nanomaterials for enhanced conductivity, and novel manufacturing techniques, all contributing to improved ASSB performance, safety, and scalability. These developments effectively tackle the limitations of traditional lithium-ion batteries, such as safety issues, limited energy density, and a reduced cycle life. Noteworthy achievements include freestanding ceramic electrolyte films like the 25 μm thick Li0.34La0.56TiO3 film, which enhance energy density and power output, and solid polymer electrolytes like the polyvinyl nitrile boroxane electrolyte, which offer improved mechanical robustness and electrochemical performance. Hybrid solid electrolytes combine the best properties of inorganic and polymer materials, providing superior ionic conductivity and mechanical flexibility. The scalable production of ultrathin composite polymer electrolytes shows promise for high-performance, cost-effective ASSBs. However, challenges remain in optimizing manufacturing processes, enhancing electrode-electrolyte interfaces, exploring sustainable materials, and standardizing testing protocols. Continued collaboration among academia, industry, and government is essential for driving innovation, accelerating commercialization, and achieving a sustainable energy future, fully realizing the transformative potential of ASSB technology for EVs and beyond.
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Thangadurai, Venkataraman. "(Invited) Lithium – Sulfur Batteries". ECS Meeting Abstracts MA2022-02, nr 4 (9.10.2022): 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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Thangadurai, Venkataraman. "(Invited) Garnet Solid Electrolytes for Advanced All-Solid-State Li Metal Batteries". ECS Meeting Abstracts MA2022-02, nr 47 (9.10.2022): 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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Zhai, Yanfang, Wangshu Hou, Zongyuan Chen, Zhong Zeng, Yongmin Wu, Wensheng Tian, Xiao Liang i in. "A hybrid solid electrolyte for high-energy solid-state sodium metal batteries". Applied Physics Letters 120, nr 25 (20.06.2022): 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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Gerstenberg, Jessica, Dominik Steckermeier, Arno Kwade i Peter Michalowski. "Effect of Mixing Intensity on Electrochemical Performance of Oxide/Sulfide Composite Electrolytes". Batteries 10, nr 3 (7.03.2024): 95. http://dx.doi.org/10.3390/batteries10030095.
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Despite the variety of solid electrolytes available, no single solid electrolyte has been found that meets all the requirements of the successor technology of lithium-ion batteries in an optimum way. However, composite hybrid electrolytes that combine the desired properties such as high ionic conductivity or stability against lithium are promising. The addition of conductive oxide fillers to sulfide solid electrolytes has been reported to increase ionic conductivity and improve stability relative to the individual electrolytes, but the influence of the mixing process to create composite electrolytes has not been investigated. Here, we investigate Li3PS4 (LPS) and Li7La3Zr2O12 (LLZO) composite electrolytes using electrochemical impedance spectroscopy and distribution of relaxation times. The distinction between sulfide bulk and grain boundary polarization processes is possible with the methods used at temperatures below 10 °C. We propose lithium transport through the space-charge layer within the sulfide electrolyte, which increases the conductivity. With increasing mixing intensities in a high-energy ball mill, we show an overlay of the enhanced lithium-ion transport with the structural change of the sulfide matrix component, which increases the ionic conductivity of LPS from 4.1 × 10−5 S cm−1 to 1.7 × 10−4 S cm−1.
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Kim, Ji Sook, Sun Hwa Lee i Dong Wook Shin. "Fabrication of Hybrid Solid Electrolyte by LiPF6 Liquid Electrolyte Infiltration into Nano-Porous Na2O-SiO2-B2O3 Glass Membrane". Solid State Phenomena 124-126 (czerwiec 2007): 1027–30. http://dx.doi.org/10.4028/www.scientific.net/ssp.124-126.1027.
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To improve ion mobility in solid inorganic electrolyte for lithium ion battery, the hybrid electrolytes were developed in the form of the organic-inorganic meso-scale hybridization by the infiltration of liquid electrolyte into meso-porous inorganic glass membrane. Glass electrolyte membranes with nanopores were prepared by spinodal decomposition and subsequent acid leaching. The most suitable glass electrolyte membranes could be fabricated from the 7.5Na2O-46.25B2O3 -46.25SiO2 (mol%). The effect of leaching temperature, leaching time and leaching acids on the preparation of the membranes were investigated. The microstructure of the cross-section of 7.5Na2O-46.25B2O3-46.25SiO2 glass electrolytes were examined with a scanning electron microscope. Then, liquid electrolyte was infiltrated by dipping method into etched glasses electrolyte. Full cells were fabricated by LiCoO2 for cathode materials and MCMB for anode materials. Conductivity and charge-discharge test of the porous glass electrolyte membrane was measured.
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Wang, Linsheng. "Development of Novel High Li-Ion Conductivity Hybrid Electrolytes of Li10GeP2S12 (LGPS) and Li6.6La3Zr1.6Sb0.4O12 (LLZSO) for Advanced All-Solid-State Batteries". Oxygen 1, nr 1 (15.07.2021): 16–21. http://dx.doi.org/10.3390/oxygen1010003.
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A lithium superionic conductor of Li10GeP2S12 that exhibits the highest lithium ionic conductivity among the sulfide electrolytes and the most promising oxide electrolytes, namely, Li6.6La3Sr0.06Zr1.6Sb0.4O12 and Li6.6La3Zr1.6Sb0.4O12, are successfully synthesized. Novel hybrid electrolytes with a weight ratio of Li6.6La3Zr1.6Sb0.4O12 to Li10GeP2S12 from 1/1 to 1/3 with the higher Li-ion conductivity than that of the pure Li10GeP2S12 electrolyte are developed for the fabrication of the advanced all-solid-state Li batteries.
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Kirchberger, Anna Maria, Patrick Walke i Tom Nilges. "Effect of Nanostructured Inorganic Ceramic Filler on Poly(ethylene oxide)-Based Solid Polymer Electrolytes". ECS Meeting Abstracts MA2023-01, nr 6 (28.08.2023): 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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Méry, Adrien, Steeve Rousselot, David Lepage, David Aymé-Perrot i Mickael Dollé. "Limiting Factors Affecting the Ionic Conductivities of LATP/Polymer Hybrid Electrolytes". Batteries 9, nr 2 (28.01.2023): 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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Muñoz, Bianca K., Jorge Lozano, María Sánchez i Alejandro Ureña. "Hybrid Solid Polymer Electrolytes Based on Epoxy Resins, Ionic Liquid, and Ceramic Nanoparticles for Structural Applications". Polymers 16, nr 14 (18.07.2024): 2048. http://dx.doi.org/10.3390/polym16142048.
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Solid polymer electrolytes (SPE) and composite polymer electrolytes (CPE) serve as crucial components in all-solid-state energy storage devices. Structural batteries and supercapacitors present a promising alternative for electric vehicles, integrating structural functionality with energy storage capability. However, despite their potential, these applications are hampered by various challenges, particularly in the realm of developing new solid polymer electrolytes that require more investigation. In this study, novel solid polymer electrolytes and composite polymer electrolytes were synthesized using epoxy resin blends, ionic liquid, lithium salt, and alumina nanoparticles and subsequently characterized. Among the formulations tested, the optimal system, designated as L70P30ILE40Li1MAl2 and containing 40 wt.% of ionic liquid and 5.7 wt.% of lithium salt, exhibited exceptional mechanical properties. It displayed a remarkable storage modulus of 1.2 GPa and reached ionic conductivities of 0.085 mS/cm at 60 °C. Furthermore, a proof-of-concept supercapacitor was fabricated, demonstrating the practical application of the developed electrolyte system.
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Ji, Xiaoyu, Yiruo Zhang, Mengxue Cao, Quanchao Gu, Honglei Wang, Jinshan Yu, Zi-Hao Guo i Xingui Zhou. "Advanced inorganic/polymer hybrid electrolytes for all-solid-state lithium batteries". Journal of Advanced Ceramics 11, nr 6 (13.05.2022): 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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Giffin, Guinevere A., Mara Goettlinger, Hendrik Bohn, Simone Peters, Mario Weller, Alexander Naßmacher, Timo Brändel i Alex Friesen. "Development of a Polymer-Based Silicon-NMC Solid-State Cell". ECS Meeting Abstracts MA2023-02, nr 2 (22.12.2023): 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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Ryu, Kun, Kyungbin Lee, Hyun Ju, Jinho Park, Ilan Stern i Seung Woo Lee. "Ceramic/Polymer Hybrid Electrolyte with Enhanced Interfacial Contact for All-Solid-State Lithium Batteries". ECS Meeting Abstracts MA2022-02, nr 7 (9.10.2022): 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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Yan, Shuo, Chae-Ho Yim, Ali Merati, Elena A. Baranova, Yaser Abu-Lebdeh i Arnaud Weck. "Interfacial Challenge for Solid-State Lithium Batteries- Liquid Addition". ECS Meeting Abstracts MA2023-01, nr 6 (28.08.2023): 1010. http://dx.doi.org/10.1149/ma2023-0161010mtgabs.
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All solid-state lithium batteries with garnet electrolytes (Li7La3Zr2O12, LLZO) are promising energy storage devices that have gained increasing attention due to their huge potential towards non-flammability and higher energy density. However, reported solid-state lithium batteries cannot achieve the projected energy density (> 500 Wh/kg at the cell level) mainly due to insufficient contact and poor compatibility between LLZO and electrodes. The use of liquid electrolytes in small quantities has been suggested as a component in the quasi-solid hybrid electrolytes to address these two issues. However, the working principle of liquid electrolytes added as the interface inside the batteries is not clear yet. This study added 10L carbonate-based liquid electrolyte between LLZO and LiNi0.6Mn0.6Co0.2O2 (NMC 622) cathode. The assembled Li|LLZO|NMC 622 cell exhibited an initial discharge capacity of 168 mAh g-1 with a capacity retention ratio of ~82 % after 28 cycles. Scanning Transmission X-ray Microscopy revealed the reaction of LE with garnet and NMC 622. More importantly, the LE decomposed and solidified during the cycling process. Decomposed LE participated in the formation of a newly-identified solid-liquid electrolyte interface (SLEI) just after the 1st cycle. Furthermore, the X-ray Absorption Spectroscopy results indicated that the SLEI consisted predominantly of LiF, LaF3, Li2O, and Li2CO3 species. Overall, this study proved the solidification of liquid electrolytes at the garnet/cathode interface. The formation of SLEI effectively suppressed the degradation of the garnet electrolyte and stabilized the battery cycling performance. More efforts are required to optimize the liquid and establish a more stable SLEI that could expand the cycling life of the batteries.
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Zhang, L. X., Y. Z. Li, L. W. Shi, R. J. Yao, S. S. Xia, Y. Wang i Y. P. Yang. "Electrospun Polyethylene Oxide (PEO)-Based Composite polymeric nanofiber electrolyte for Li-Metal Battery". Journal of Physics: Conference Series 2353, nr 1 (1.10.2022): 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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Lee, Yan Ying, i Andre Weber. "Harmonization of Testing Procedures for All Solid State Batteries". ECS Meeting Abstracts MA2023-02, nr 2 (22.12.2023): 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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Yan, Shuo, Chae-Ho Yim, Vladimir Pankov, Mackenzie Bauer, Elena Baranova, Arnaud Weck, Ali Merati i Yaser Abu-Lebdeh. "Perovskite Solid-State Electrolytes for Lithium Metal Batteries". Batteries 7, nr 4 (7.11.2021): 75. http://dx.doi.org/10.3390/batteries7040075.
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Solid-state lithium metal batteries (LMBs) have become increasingly important in recent years due to their potential to offer higher energy density and enhanced safety compared to conventional liquid electrolyte-based lithium-ion batteries (LIBs). However, they require highly functional solid-state electrolytes (SSEs) and, therefore, many inorganic materials such as oxides of perovskite La2/3−xLi3xTiO3 (LLTO) and garnets La3Li7Zr2O12 (LLZO), sulfides Li10GeP2S12 (LGPS), and phosphates Li1+xAlxTi2−x(PO4)3x (LATP) are under investigation. Among these oxide materials, LLTO exhibits superior safety, wider electrochemical window (8 V vs. Li/Li+), and higher bulk conductivity values reaching in excess of 10−3 S cm−1 at ambient temperature, which is close to organic liquid-state electrolytes presently used in LIBs. However, recent studies focus primarily on composite or hybrid electrolytes that mix LLTO with organic polymeric materials. There are scarce studies of pure (100%) LLTO electrolytes in solid-state LMBs and there is a need to shed more light on this type of electrolyte and its potential for LMBs. Therefore, in our review, we first elaborated on the structure/property relationship between compositions of perovskites and their ionic conductivities. We then summarized current issues and some successful attempts for the fabrication of pure LLTO electrolytes. Their electrochemical and battery performances were also presented. We focused on tape casting as an effective method to prepare pure LLTO thin films that are compatible and can be easily integrated into existing roll-to-roll battery manufacturing processes. This review intends to shed some light on the design and manufacturing of LLTO for all-ceramic electrolytes towards safer and higher power density solid-state LMBs.
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Shah, Vaidik, i 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, nr 4 (22.12.2023): 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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Tsurumaki, Akiko, Rossella Rettaroli, Lucia Mazzapioda i Maria Assunta Navarra. "Inorganic–Organic Hybrid Electrolytes Based on Al-Doped Li7La3Zr2O12 and Ionic Liquids". Applied Sciences 12, nr 14 (21.07.2022): 7318. http://dx.doi.org/10.3390/app12147318.
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Organic–inorganic hybrid electrolytes based on Al-doped Li7La3Zr2O12 (LLZO) and two different ionic liquids (ILs), namely N-ethoxyethyl-N-methylpiperidinium bis(fluorosulfonyl)imide (FSI IL) and N-ethoxyethyl-N-methylpiperidinium difluoro(oxalato)borate (DFOB IL), were prepared with the aim of improvement of inherent flexibilities of inorganic solid electrolytes. The composites were evaluated in terms of thermal, spectroscopical, and electrochemical properties. In the impedance spectra of LLZO composites with 15 wt% ILs, a semi-circle due to grain boundary resistances was not observed. With the sample merely pressed with 1 ton, without any high-temperature sintering process, the ionic conductivity of 10−3 S cm−1 was achieved at room temperature. Employing a ternary composite of LLZO, FSI IL, and LiFSI as an electrolyte, all-solid-state lithium metal batteries having LiFePO4 as a cathode were assembled. The cell exhibited a capacity above 100 mAh g−1 throughout the course of charge–discharge cycle at C/20. This confirms that FSI IL is an effective additive for inorganic solid electrolytes, which can guarantee the ion conduction.
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Jiang, Wen, Lingling Dong, Shuanghui Liu, Bing Ai, Shuangshuang Zhao, Weimin Zhang, Kefeng Pan i Lipeng Zhang. "Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride Layer". Nanomaterials 12, nr 12 (12.06.2022): 2023. http://dx.doi.org/10.3390/nano12122023.
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The next generation of all-solid-state batteries can feature battery safety that is unparalleled among conventional liquid batteries. The garnet-type solid-state electrolyte Li7La3Zr2O12 (LLZO), in particular, is widely studied because of its high Li-ion conductivity and stability in air. However, the poor interface-contact between Li and the electrolyte (garnet) severely limits the development of solid electrolytes. In this study, we synthesize cubic phase Li6.4La3Zr1.4Ta0.6O12 (LLZTO) using a secondary sintering method. In addition, a thin aluminum nitride (AlN) layer is introduced between the metal (Li) and the solid electrolyte. Theoretical calculations show that AlN has a high affinity for Li. Furthermore, it is shown that the AlN coating can effectively reduce the interface impedance between Li and the solid electrolyte and improve the lithium-ion transport. The assembled symmetric Li cells can operate stably for more than 3600 h, unlike the symmetric cells without AlN coating, which short-circuited after only a few cycles. The hybrid solid-state battery with a modified layer, which is assembled using LiFePO4 (LFP), still has a capacity of 120 mAh g−1 after 200 cycles, with a capacity retention rate of 98%. This shows that the introduction of an AlN interlayer is very helpful to obtain a stable Li/solid-electrolyte interface, which improves the cycling stability of the battery.
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Teshima, Katsuya, Hajime Wagata i Shuji Oishi. "All-Crystal-State Lithium-Ion Batteries: Innovation Inspired by Novel Flux Coating Method." Additional Conferences (Device Packaging, HiTEC, HiTEN, and CICMT) 2013, CICMT (1.09.2013): 000187–91. http://dx.doi.org/10.4071/cicmt-wp41.
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All-solid-state lithium-ion rechargeable batteries (LIBs) consisting of solid electrolyte materials have attracted a number of research interests because no use of organic liquid electrolyte increases packaging density and intrinsic safety of LIB, which contribute the development on environmentally-friendly automobiles such as electric vehicle (EV), hybrid vehicle (HV), and plug-in hybrid vehicle (HEV), in addition to efficient utilization of electric energy in smart grid. Among various solid electrolytes, inorganic electrolyte materials have achieved relatively high lithium-ion conductivity and better stability at an ambient atmosphere. Nevertheless, there is a drawback that is relatively high internal resistance owing to relatively slow Li ion movement caused by low crystallinity of materials, scattering at interfaces such as current collector/electrode active materials and electrode active materials/electrolyte materials. In this context, we have proposed a concept, all-crystal-state LIB, in which all the component materials have high crystallinity and those interfaces are effective for Li ion diffusion. Here, we present the fabrication of oxide crystals and crystal layers via flux method and flux coating. Flux method is one of the solution processes in which idiomorphic highly crystalline materials can be obtained under the melting point of the target ones. In addition, it provides simple, low-cost and environmentally-benign pathway compared to conventional solid-state-reaction method. Flux coating method is developed to fabricate high-quality crystal layers (films) on various substrates. High-quality crystals and crystal layers of cathode, anode and electrolyte materials were successfully fabricated.
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Babkova, Tatiana, Rudolf Kiefer i 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, nr 4 (19.02.2024): 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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Karahan Toprakci, Hatice Aylin, i Ozan Toprakci. "Recent Advances in New-Generation Electrolytes for Sodium-Ion Batteries". Energies 16, nr 7 (31.03.2023): 3169. http://dx.doi.org/10.3390/en16073169.
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Sodium-ion batteries (SIBs) are one of the recent trends in energy storage systems due to their promising properties, the high abundance of sodium in the Earth’s crust, and their low cost. However, the commercialization process of SIBs is in the early stages of development because of some challenges related to electrodes and electrolytes. Electrolytes are vital components of secondary batteries because they determine anode/cathode performance; energy density; operating conditions (electrochemical stability window, open circuit voltage, current rate, etc.); cyclic properties; electrochemical, thermal, mechanical, and dimensional stability; safety level; and the service life of the system. The performance of the battery is based on the structural, morphological, electrical, and electrochemical properties of the electrolytes. In this review, electrolytes used for SIBs are classified according to their state and material, including liquid, quasi-solid, solid, and hybrid, and recent advances in electrolyte research have been presented by considering their contributions and limitations. Additionally, future trends and recent cutting-edge research are highlighted.
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Okos, Alexandru, Cristina Florentina Ciobota, Adrian Mihail Motoc i Radu-Robert Piticescu. "Review on Synthesis and Properties of Lithium Lanthanum Titanate". Materials 16, nr 22 (8.11.2023): 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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Lisovskyi, Ivan, Mykyta Barykin, Sergii Solopan i Anatolii Belous. "FEATURES OF PHASE TRANSFORMATIONS IN THE SYNTHESIS OF COMPLEX LITHIUM-CONDUCTING OXIDE MATERIALS". Ukrainian Chemistry Journal 87, nr 9 (25.10.2021): 14–34. http://dx.doi.org/10.33609/2708-129x.87.09.2021.14-34.
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Lithium-ion batteries (LIB`s) are widely used in consumer electronics, mobile phones, personal computers, as well as in hybrid and electric vehicles. Liquid electrolytes, which mainly consist of aprotic organic solvents and lithium-conductive salts, are used for the transfer of lithium ions in LIB`s. However, the application of liquid electrolytes in LIB`s leads to a number of problems, the most significant of which are the risk of battery ignition during operation due to the presence of flammable organic solvents and loss of capacity due to the interaction of liquid electrolyte with electrode materials during cycling. An alternative that can ensure the safety and reliability of lithium batteries is the development of completely solid state batteries (SSB`s). SSB`s are not only inherently safer due to the absence of flammable organic components, but also have the potential to increase significantly the energy density. Instead of a porous separator based on polypropylene saturated with a liquid electrolyte, the SSB`s use a solid electrolyte that acts as an electrical insulator and an ionic conductor at the same time. The use of a compact solid electrolyte, which acts as a physical barrier that prevents the growth of lithium dendrites, also allows using lithium metal as the anode material.
It is desirable to use oxide systems as the solid electrolytes for SSB`s, as they are resistant to moisture and atmospheric air. Among the lithium-conducting oxide materials, which exhibit relatively high lithium conductivity at a room temperature and can be used as a solid electrolyte in the completely solid-state batteries, lithium-air batteries and other electrochemical devices, the most promising materials are ones with NASICON, perovskite and garnet-type structures.
The phase transformations that occur during the synthesis of complex lithium-conductive oxides, namely Li1.3Al0.3Ti1.7(PO4)3 with the NASICON-type structure, Li0.34La0.56TiO3 with the perovskite-type structure and Li6.5La3Zr1.5Nb0.5O12 with the garnet-type structure by the solid-state reactions method in an air were investigated. The optimal conditions for the synthesis of each of the above-mentioned compounds were determined.
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Lin, Ruifan, Yingmin Jin, Yumeng Li, Xuebai Zhang i Yueping Xiong. "Recent Advances in Ionic Liquids—MOF Hybrid Electrolytes for Solid-State Electrolyte of Lithium Battery". Batteries 9, nr 6 (6.06.2023): 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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Liu, Yue, Qintao Sun, Peiping Yu, Bingyun Ma, Hao Yang, Jiayi Zhang, Miao Xie i Tao Cheng. "In situ formation of circular and branched oligomers in a localized high concentration electrolyte at the lithium-metal solid electrolyte interphase: a hybrid ab initio and reactive molecular dynamics study". Journal of Materials Chemistry A 10, nr 2 (2022): 632–39. http://dx.doi.org/10.1039/d1ta08182a.
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Developing advanced electrolytes has been considered as a promising approach to stabilize the lithium metal anode via the formation of a stable solid electrolyte interphase (SEI) that can protect the Li anode to enable long-term cycling stability.
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Toghyani, Somayeh, Florian Baakes, Ningxin Zhang, Helmut Kühnelt, Walter Cistjakov i 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, nr 4 (9.10.2022): 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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Thangadurai, Venkataraman, Sanoop Palakkathodi Kammampata i Hirotoshi Yamada. "(Invited) Garnet-Type Electrolytes for All-Solid-State Lithium Metal Batteries". ECS Meeting Abstracts MA2022-02, nr 1 (9.10.2022): 37. http://dx.doi.org/10.1149/ma2022-02137mtgabs.
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All solid-state Li batteries are foreseen as the future state of battery technology due to their safety, high energy density, and high potential window as compared to the present organic liquid electrolyte batteries. Li-ion conducting garnet-type electrolytes have received considerable research interests due to their compatibility with Li metal anode, good ionic conductivity (10-3 S/cm) and wide electrochemical window (~ 6V vs. Li).1 Garnet-type Li6.5La3-xAxZr1.5-xTax+0.5O12 (A = Ca, Sr, Ba; x = 0.1, 0.5) solid electrolytes were prepared by conventional solid-state synthesis and spark plasma synthesis (SPS).2-4 The formation of the cubic garnet-type structure was confirmed by powder X-ray diffraction (PXRD). Microstructure of the solid electrolytes were analysed by scanning electron microscopy (SEM) and cross-sectional analyses showed that the SPS processed samples are highly dense compared to the same compositions prepared by conventional solid-state route. The AC electrochemical impedance spectroscopy (EIS) was used to measure the impedance of solid electrolytes and found that all samples exhibit bulk conductivity in the order of 10-4 S/cm at room temperature. SPS processed samples showed an excellent Li-ion charge transfer resistance and the highest critical current density compared to the samples prepared by conventional solid-state synthesis. X-ray photoelectron spectroscopy (XPS) analyses were conducted on SPS-processed samples to quantify the impurity layers on garnet surface. Electrochemical performance of a hybrid cell consisting of liquid Li-ion electrolytes and garnet electrolyte will be discussed. References Wang, K. Fu, S. Palakkathodi Kammampata, D. W. McOwen, A. Junio Samson, L. Zhang, G. T. Hitz, A. M. Nolan, E. D. Wachsman, Y. Mo, V. Thangadurai and L. Hu, Chem. Rev., 2020, 120, 4257–4300. Palakkathodi Kammampata, R. H. Basappa, T. Ito, H. Yamada and V. Thangadurai, ACS Appl. Energy Mater., 2019, 2, 1765–1773. Palakkathodi Kammampata, H. Yamada, T. Ito, R. Paul and V. Thangadurai, J. Mater. Chem. A, 2020, 8, 2581–2590. Yamada, T. Ito, S. P. Kammampata and V. Thangadurai, ACS Appl. Mater. Interfaces, 2020, 12, 36119–36127.
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Bertrand, Marc, Steeve Rousselot, David Aymé-Perrot i Mickaël Dollé. "Assembling an All-Solid-State Ceramic Battery: Assessment of Chemical and Thermal Compatibility of Solid Ceramic Electrolytes and Active Material Using High Temperature X-Ray Diffraction". ECS Meeting Abstracts MA2022-02, nr 7 (9.10.2022): 2421. http://dx.doi.org/10.1149/ma2022-0272421mtgabs.
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Lithium ion batteries (LIBs) are the most known and used batteries for portable energy storage because of their high energy densities, long cycle life and relatively low price. However, they still fall short for the development of long range electric vehicles and stationary applications due to organic liquid electrolytes that are currently electrochemically limited and present safety issues (fire or explosion in case of short-cut or overcharging). Solid oxide electrolytes appear to be one of the solutions because of their non-flammability and wide potential window. Inorganic oxide electrolytes have reasonable ionic conductivities (10-5-10-3 S/cm at ambient temperature), high mechanical strength, and high chemical stability. Assembling an all ceramic solid-state battery with inorganic oxide electrolyte is challenging as it requires a deep knowledge of the thermal, chemical and electrochemical behavior of each component of the cell. The battery must be a continuous monolithic block with a thin dense electrolyte separator, in order to minimize the polarization. In addition, optimized interfaces between active material and electrolytes must be ensured in the composite electrodes. This is often achieved with oxide-based materials by using high temperature processing. Thermal expansion occurring during this step can lead to cracks, which will affect the performance and cyclability of the device. The primary driving force of a crack during the fabrication of hybrid ceramic is the stress due to mismatch in the coefficient of thermal expansion (TEC) of the various layers/materials. Moreover, it must be certain that no reaction occurs between active material and electrolytes in the sintering temperature range. These are then two key parameters to address for the development of all ceramic solid-state batteries. In this work, in situ-XRD has been used to determine the TEC and the thermal stability of various well-known oxide active materials and solid electrolytes. The aim of this presentation is to discuss about the best selection of compatible oxide-based materials to avoid unwanted cracks or reaction during the sintering processing of ceramic solid-state batteries.
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Loudeche, Maxime, Rémy Rouxhet i Joris Proost. "Development of a New Type of Electrochemical Reactor for Low Temperature Lime and Cement Production". ECS Meeting Abstracts MA2023-01, nr 24 (28.08.2023): 1603. http://dx.doi.org/10.1149/ma2023-01241603mtgabs.
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The cement industry is responsible for more than 8% of the global CO2 emissions, making it one of the largest contributors to global warming. Two-thirds of these emissions are coming from unavoidable process gases caused by the calcination reaction of limestone (CaCO3). The remaining emissions are mainly coming from the combustion of fossil fuels. Due to the high temperature requirement (≈1500°C), direct electrification is difficult to consider. For these two reasons, the cement industry is therefore known as a challenging sector to decarbonize. A new electrochemical pathway for cement production has gained prominence in the scientific literature in recent years [1]. This technology has the potential to electrify the cement and lime production while producing at the same time valuable gases (O2, CO2, H2). It is based on a new type of hybrid electrolyser capable of working with solid, liquid and gaseous phases. Thanks to the acidity generated by water oxidation at the anode, the solid limestone feed, precursor of cement, is being dissolved. This dissolution produces pure CO2 which is mixed with pure O2 generated by electrolysis and which is easily captured for later use. The calcium ions are then migrating towards the cathode under the effect of the electric field. The OH- hydroxyl ions, produced at the cathode by water reduction, meet the calcium ions to form the final solid product, hydrated lime (Ca(OH)2). This lime can be used as such or converted into cement by additional steps. In this research, a laboratory-scale setup has been developed to study the feasibility of such a process. Different geometries have been tested and the main operational parameters affecting the different steps of the process have been investigated. Our results show first of all the formation and stabilization of a pH gradient within the electrolyser, which allows at the same time for the complete dissolution of CaCO3 in the acidic anodic environment while producing a white precipitate of Ca(OH)2 at the cathode. The setup also presents ideal faradaic efficiencies when using an IrO2 coated titanium anode and a nickel cathode in a 1M NaClO4 electrolyte. Alternative electrode materials, including a 316L stainless steel anode and an Inconel 718 cathode, have been considered as well. Finally, it was shown that the energetic efficiency can be further improved by pushing the kinetics of the dissolution and precipitation reactions through increasing the mobility of calcium ions, using Ca-based electrolytes, like Ca(ClO4)2. Based on our results, all the elementary concepts behind the hybrid electrolyser have been established, and a first blueprint of a continuous industrial process will be proposed. [1] - L. D. Ellis, et al. (2019). Toward electrochemical synthesis of cement—An electrolyzer-based process for decarbonating CaCO3 while producing useful gas streams. PNAS , 117, 12584-12591. Figure 1
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Berling, Sabrina, Jose Manuel Hidalgo, Sotirios Mavrikis, Nagaraj Patil, Enrique Garcia - Quismondo, Jesus Palma i Carlos Ponce de Leon. "Adaptation of a Vanadium Redox Flow Battery for Thermal Applications Using a Solid Capacity Booster". ECS Meeting Abstracts MA2023-02, nr 59 (22.12.2023): 2851. http://dx.doi.org/10.1149/ma2023-02592851mtgabs.
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In this work a novel approach for the use of the Vanadium Redox Flow Batteries (VRFB) is made by viewing it as a dual system with the ability to store both electrical and thermal energy. Electrical energy is thanks to the electrochemical reactions of the vanadium ions dissolved in the electrolyte, while thermal energy will use the sensible heat of the electrolyte mass. The performance of VRFB has been widely studied over the last 40 years and there is an extensive bibliography on the subject regarding the electrochemical performance attending only to the conventional energy storage requirements, but the hybrid electrical-thermal function is a novel subject that has been scarcely explored. One of the most critical aspects is the narrow operating temperature range of these batteries (15-40°C) that strongly limits their thermal energy storage capacity. Practical vanadium electrolytes operate with electrolytes containing a vanadium concentration between 1.6 and 2.0 M, and usually also employ cooling and heating systems to maintain the temperature between 15 and 40ºC. In particular, at temperatures below 15ºC the slower reaction kinetics, high viscosity and reduced conductivity of the concentrated electrolytes introduce remarkable energy losses in the battery. On the other hand, at temperatures over 35ºC the positive electrolyte is not stable due to the limited solubility of VO2 + species. High temperatures also boost the kinetics of parasitic reactions such as hydrogen and oxygen evolution, thus increasing energy losses. In this study, we address these limitations aiming to open up new possibilities of a successful integration of vanadium redox flow batteries into thermal applications. For this, the functionality and stability limits of a diluted vanadium electrolyte are analyzed for an extended operational temperature window from 5ºC to 50ºC and compared to commercial electrolyte formulations. In a second step, the use of a solid capacity booster is investigated to compensate the loss of energy density due to electrolyte dilution. [1] S. Berling, S. Mavrikis, N. Patil, E. García – Quismondo, J. Palma, C. Ponce de León “Lignin as redox-targeted catalyst for the positive vanadium electrolyte”, Electrochemistry Communications 142 (2022) 107339. [2] S. Berling, J. M. Hidalgo, N. Patil, E. García - Quismondo, J. Palma, C.Ponce de León, “A mediated vanadium flow battery: Lignin as redox-targeting active material in the vanadium catholyte”. Submitted
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Lim, Seung, Juyoung Moon, Uoon Baek, Jae Lee, Youngjin Chae i Jung Park. "Shape-Controlled TiO2 Nanomaterials-Based Hybrid Solid-State Electrolytes for Solar Energy Conversion with a Mesoporous Carbon Electrocatalyst". Nanomaterials 11, nr 4 (3.04.2021): 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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Tam, Vincent, i Jesse S. Wainright. "Considerations for Ionic Diffusion in Slurry Electrolytes for Redox Flow Batteries". ECS Meeting Abstracts MA2023-01, nr 3 (28.08.2023): 784. http://dx.doi.org/10.1149/ma2023-013784mtgabs.
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Slurry electrodes have been proposed as a means to enhance the scalability of hybrid redox flow battery (RFB) chemistries for better usability in utility scale energy storage applications1–3. In conventional hybrid RFB’s, scalability is limited due the spatial constraints of the flow cell and the metal deposited by the negative half-reaction on charge1. By using a slurry electrode, the solid metal can be deposited onto electrically conductive particles dispersed in the electrolyte instead of on the stationary electrode within the flow cell. In this way, hybrid RFB chemistries can achieve the same scalability as more commonly studied true RFB chemistries, such as all-vanadium. Due to the high abundance, low cost, and low toxicity of iron electrolytes, the all-iron RFB chemistry is of particular interest for use with a slurry electrode2,4. The usefulness of the slurry electrode depends on the current distribution of the plating reaction. To successfully decouple the storage and power capacities of the RFB and thus enhance its scalability5, the faradaic current of the plating reaction must occur predominantly on the mobile slurry particles, as opposed to on the stationary current collector1. This current distribution is dependent on a variety of factors, such as the applied overpotential, the electrical conductivity of the slurry, the ionic conductivity of the electrolyte, the kinetics of the reaction, and the rate of ionic mass transport to reaction sites. Ionic mass transport in electrolytes containing slurry electrodes may differ from ionic transport in neat electrolyte in interesting and important ways. Due to the volume fraction of the electrolyte occupied by solid particles, the effective concentration of the ionic species may be lower than in neat electrolyte. Further, the solid particle volume fraction hinders ionic diffusion by introducing diffusion path tortuosity. This effect is more severe in higher slurry particle loadings. In this work, the effect of varying dispersed solid particle loading on ionic diffusivity is investigated via voltammetry using a rotating disk electrode. The diffusivities of ionic iron species are measured as a function of the volume fraction of solids dispersed in the electrolyte. Comparisons with the Bruggeman correlation6,7 are made and amendments to the Levich equation are considered. (1) Petek, T. J.; Hoyt, N. C.; Savinell, R. F.; Wainright, J. S. Slurry Electrodes for Iron Plating in an All-Iron Flow Battery. J. Power Sources 2015, 294, 620–626. https://doi.org/10.1016/j.jpowsour.2015.06.050. (2) Petek, T. J. Enhancing the Capacity of All-Iron Flow Batteries: Understanding Crossover and Slurry Electrodes. Ph.D. Thesis 2015, No. May. (3) Narayanan, T. M.; Zhu, Y. G.; Gençer, E.; McKinley, G.; Shao-Horn, Y. Low-Cost Manganese Dioxide Semi-Solid Electrode for Flow Batteries. Joule 2021, 5 (11), 2934–2954. https://doi.org/10.1016/j.joule.2021.07.010. (4) Dinesh, A.; Olivera, S.; Venkatesh, K.; Santosh, M. S.; Priya, M. G.; Inamuddin; Asiri, A. M.; Muralidhara, H. B. Iron-Based Flow Batteries to Store Renewable Energies. Environ. Chem. Lett. 2018, 16 (3), 683–694. https://doi.org/10.1007/s10311-018-0709-8. (5) Weber, A. Z.; Mench, M. M.; Meyers, J. P.; Ross, P. N.; Jeffrey, T.; Liu, Q. Redox Flow Batteries , a Review Environmental Energy Technologies Division , Lawrence Berkeley National Laboratory , Department of Mechanical , Aerospace and Biomedical Engineering , University of Tennessee , Department of Chemical Engineering , McGill Un. 1–72. (6) Tjaden, B.; Cooper, S. J.; Brett, D. J.; Kramer, D.; Shearing, P. R. On the Origin and Application of the Bruggeman Correlation for Analysing Transport Phenomena in Electrochemical Systems. Curr. Opin. Chem. Eng. 2016, 12, 44–51. https://doi.org/10.1016/j.coche.2016.02.006. (7) Chung, D. W.; Ebner, M.; Ely, D. R.; Wood, V.; Edwin García, R. Validity of the Bruggeman Relation for Porous Electrodes. Model. Simul. Mater. Sci. Eng. 2013, 21 (7). https://doi.org/10.1088/0965-0393/21/7/074009.
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Sankara Raman, Ashwin, Samik Jhulki, Billy Johnson, Aashray Narla i Gleb Yushin. "Facile in-Situ Polymerized Polymer Electrolytes in All Solid-State Lithium-Ion Batteries". ECS Meeting Abstracts MA2022-02, nr 3 (9.10.2022): 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.