Journal articles on the topic 'Electrolyte hybride'
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1
Kanai, Yamato, Koji Hiraoka, Mutsuhiro Matsuyama, and Shiro Seki. "Chemically and Physically Cross-Linked Inorganic–Polymer Hybrid Solvent-Free Electrolytes." Batteries 9, no. 10 (September 26, 2023): 492. http://dx.doi.org/10.3390/batteries9100492.
Abstract:
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.
2
Byeon, Sang Sik, Kai Wang, Chan Gyu Lee, Yeon Gil Jung, and Bon Heun Koo. "Effect of Phosphate and Nitrate Electrolytes on Growth of Ceramic Coatings on 2021 Al Alloys Prepared by Electrolytic Plasma Processing." Advanced Materials Research 123-125 (August 2010): 1035–38. http://dx.doi.org/10.4028/www.scientific.net/amr.123-125.1035.
Abstract:
2021 series aluminum alloy is used as the matrix material for its wide application in engineering to make AlON coating layers by the electrolytic plasma processing (EPP) method. The experiments were carried out on 2021 Al alloys in alkaline electrolytes which are eco-friendly and low-cost. The experimental electrolyte composition includes: 2g/L NaOH as the electrolytic conductive agent, 6~14g/L Na3PO4 as alumina formative agent, 0.5g/L NaNO3 as a nitrogen inducing agent. The effects of phosphate content variation are evaluated by a combined composition and structure analysis of the coating layer using with Philips-X’Pert X-ray diffractometer, JSM 5610 scanning electron microscopy for the specimens EPP-treated at room temperature in 10 min under a hybrid voltage (260V DC + 200V AC-50Hz). In addition, microhardness of the ceramic coatings was measured to correlate the evolution of microstructure and resulting mechanical properties. The wear tests show that a composite of AlON-Al2O3 high anti-abrasive coating formed as a result of a reactive process between Al in the alloy itself and O-N supplied by the electrolyte.
3
LI, X. D., X. J. YIN, C. F. LIN, D. W. ZHANG, Z. A. WANG, Z. SUN, and S. M. HUANG. "INFLUENCE OF I2 CONCENTRATION AND CATIONS ON THE PERFORMANCE OF QUASI-SOLID-STATE DYE-SENSITIZED SOLAR CELLS WITH THERMOSETTING POLYMER GEL ELECTROLYTE." International Journal of Nanoscience 09, no. 04 (August 2010): 295–99. http://dx.doi.org/10.1142/s0219581x10006831.
Abstract:
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).
4
An, Yongling, Huifang Fei, Jinkui Feng, Lijie Ci, and Shenglin Xiong. "A novel Lithium/Sodium hybrid aqueous electrolyte for hybrid supercapacitors based on LiFePO4 and activated carbon." Functional Materials Letters 09, no. 06 (December 2016): 1642008. http://dx.doi.org/10.1142/s179360471642008x.
Abstract:
A novel low cost Na[Formula: see text]/Li[Formula: see text] hybrid electrolyte was proposed for hybrid supercapacitor. By partly substituting Lithium salt with Sodium salt, the Li[Formula: see text]/Na[Formula: see text] hybrid electrolyte exhibits synergic advantages of both Li[Formula: see text] and Na[Formula: see text] electrolytes. Our findings could also be applied to other hybrid power sources.
5
WANG, KAI, SANGSIK BYUN, CHAN GYU LEE, BON HEUN KOO, YI QI WANG, and JUNG IL SONG. "MICROSTRUCTURES AND ABRASIVE PROPERTIES OF THE OXIDE COATINGS ON Al6061 ALLOYS PREPARED BY PLASMA ELECTROLYTIC OXIDATION IN DIFFERENT ELECTROLYTES." Surface Review and Letters 17, no. 03 (June 2010): 271–76. http://dx.doi.org/10.1142/s0218625x1001359x.
Abstract:
Al 2 O 3 coatings were prepared on T6-tempered Al6061 alloys substrate under a hybrid voltage (AC 200 V–60 Hz and DC 260 V value) by plasma electrolytic oxidation (PEO) in 30 min. The effects of different electrolytes on the abrasive behaviors of the coatings were studied by conducting dry ball-on-disk wear tests. X-ray diffraction (XRD) and scanning electron microscopy (SEM) were used to investigate the coating microstructure. XRD analysis results show that the coatings mainly consist of α- and γ- Al 2 O 3, and some mullite and AlPO 4 phase in Na 2 SiO 3 and Na 3 PO 4 containing electrolytes, respectively. The wear test results show that the coatings which were PEO-treated in Na 3 PO 4 containing electrolyte presented the most excellent abrasive resistance property.
6
Choi, Kyoung Hwan, Eunjeong Yi, Kyeong Joon Kim, Seunghwan Lee, Myung-Soo Park, Hansol Lee, and Pilwon Heo. "(Invited) Pragmatic Approach and Challenges of All Solid State Batteries: Hybrid Solid Electrolyte for Technical Innovation." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 988. http://dx.doi.org/10.1149/ma2023-016988mtgabs.
Abstract:
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]
7
Liao, Cheng Hung, Chia-Chin Chen, Ru-Jong Jeng, and Nae-Lih (Nick) Wu. "Application of Artificial Interphase on Ni-Rich Cathode Materials Via Hybrid Ceramic-Polymer Electrolyte in All Solid State Batteries." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 1050. http://dx.doi.org/10.1149/ma2023-0161050mtgabs.
Abstract:
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
8
Villaluenga, Irune, Kevin H. Wujcik, Wei Tong, Didier Devaux, Dominica H. C. Wong, Joseph M. DeSimone, and Nitash P. Balsara. "Compliant glass–polymer hybrid single ion-conducting electrolytes for lithium batteries." Proceedings of the National Academy of Sciences 113, no. 1 (December 22, 2015): 52–57. http://dx.doi.org/10.1073/pnas.1520394112.
Abstract:
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.
9
Woolley, Henry Michael, and Nella Vargas-Barbosa. "Electrochemical Characterization of Thiophosphate- Ionic Liquid Hybrid Lithium Electrolytes Against Li Metal." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 986. http://dx.doi.org/10.1149/ma2023-016986mtgabs.
Abstract:
(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.
10
Zaman, Wahid, Nicholas Hortance, Marm B. Dixit, Vincent De Andrade, and Kelsey B. Hatzell. "Visualizing percolation and ion transport in hybrid solid electrolytes for Li–metal batteries." Journal of Materials Chemistry A 7, no. 41 (2019): 23914–21. http://dx.doi.org/10.1039/c9ta05118j.
11
Kim, Ji Sook, Sun Hwa Lee, and 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 (June 2007): 1027–30. http://dx.doi.org/10.4028/www.scientific.net/ssp.124-126.1027.
Abstract:
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.
12
Gu, Sui, Xiao Huang, Qing Wang, Jun Jin, Qingsong Wang, Zhaoyin Wen, and Rong Qian. "A hybrid electrolyte for long-life semi-solid-state lithium sulfur batteries." Journal of Materials Chemistry A 5, no. 27 (2017): 13971–75. http://dx.doi.org/10.1039/c7ta04017b.
13
Issa, Sébastien, Roselyne Jeanne-Brou, Sumit Mehan, Didier Devaux, Fabrice Cousin, Didier Gigmes, Renaud Bouchet, and Trang N. T. Phan. "New Crosslinked Single-Ion Silica-PEO Hybrid Electrolytes." Polymers 14, no. 23 (December 6, 2022): 5328. http://dx.doi.org/10.3390/polym14235328.
Abstract:
New single-ion hybrid electrolytes have been synthetized via an original and simple synthetic approach combining Michael addition, epoxidation, and sol–gel polycondensation. We designed an organic PEO network as a matrix for the lithium transport, mechanically reinforced thanks to crosslinking inorganic (SiO1.5) sites, while highly delocalized anions based on lithium vinyl sulfonyl(trifluoromethane sulfonyl)imide (VSTFSILi) were grafted onto the inorganic sites to produce single-ion hybrid electrolytes (HySI). The influence of the electrolyte composition in terms of the inorganic/organic ratio and the grafted VSTFSILi content on the local structural organization, the thermal, mechanical, and ionic transport properties (ionic conductivity, transference number) are studied by a variety of techniques including SAXS, DSC, rheometry, and electrochemical impedance spectroscopy. SAXS measurements at 25 °C and 60 °C reveal that HySI electrolyte films display locally a spatial phase separation with domains composed of PEO rich phase and silica/VSTFSILi clusters. The size of these clusters increases with the silica and VSTFSILi content. A maximum ionic conductivity of 2.1 × 10−5 S·cm−1 at 80 °C has been obtained with HySI having an EO/Li ratio of 20. The Li+ ion transfer number of HySI electrolytes is high, as expected for a single-ion electrolyte, and comprises between 0.80 and 0.92.
14
Lv, Wenjing, Kaidong Zhan, Xuecheng Ren, Lu Chen, and Fan Wu. "Comparing Charge Dynamics in Organo-Inorganic Halide Perovskite: Solid-State versus Solid-Liquid Junctions." Journal of Nanoelectronics and Optoelectronics 19, no. 2 (February 1, 2024): 121–28. http://dx.doi.org/10.1166/jno.2024.3556.
Abstract:
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.
15
Reber, David, Oleg Borodin, Maximilian Becker, Daniel Rentsch, Johannes H. Thienenkamp, Rabeb Grissa, Wengao Zhao, et al. "Water/Ionic Liquid/Succinonitrile Hybrid Electrolytes." ECS Meeting Abstracts MA2022-02, no. 2 (October 9, 2022): 161. http://dx.doi.org/10.1149/ma2022-022161mtgabs.
Abstract:
The water-in-salt concept has significantly improved the electrochemical stability of aqueous electrolytes, and the hybridization with organic solvents or ionic liquids has further enhanced their reductive stability.[1] Here, we open a large design space by introducing succinonitrile as a cosolvent in water/ionic liquid/succinonitrile hybrid electrolytes. Via addition of the nitrile, electrolyte performance metrics such as electrochemical stability, conductivity, or cost can be tuned, and salt solubility limits can be fully circumvented. We elucidate the solution structure of two select hybrid electrolytes and highlight the impact of each electrolyte component on the final formulation, showing that excess ionic liquid fractions decrease the lithium transport number, while excess nitrile addition reduces electrochemical stability and yields flammable electrolytes. If component ratios are tuned appropriately, high electrochemical stability is achieved and aqueous Li4Ti5O12 - LiNi0.8Mn0.1Co0.1O2 full cells show excellent cycling stability with a maximum energy density of ca. 140 Wh/kg of active material, and Coulombic efficiencies of close to 99.5% at 1C. Furthermore, strong rate performance over a wide temperature range, facilitated by the fast conformational dynamics of succinonitrile, with a capacity retention of 53% at 10C relative to 1C is observed.[2] References: [1] Becker, M.; Rentsch, D.; Reber, D.; Aribia, A.; Battaglia, C.; Kühnel, R.-S., The hydrotropic effect of ionic liquids in water‐in‐salt electrolytes. Angew. Chem. Int. Ed.. 2021, 60, 14100. [2] Reber, D.; Borodin, O.; Becker, M.; Rentsch, D.; Thienenkamp, J.H.; Grissa, R.; Zhao, W.; Aribia, A.; Brunklaus, G.; Battaglia, C.; Kühnel, R.-S., Water/Ionic Liquid/Succinonitrile Hybrid Electrolytes for Aqueous Batteries. Adv. Funct. Mater. 2022, 2112138.
16
Quan, Phung, Le Thi My Linh, Huynh Thi Kim Tuyen, Nguyen Van Hoang, Vo Duy Thanh, Tran Van Man, and Le My Loan Phung. "Safe sodium‐ion battery using hybrid electrolytes of organic solvent/pyrrolidinium ionic liquid." Vietnam Journal of Chemistry 59, no. 1 (February 2021): 17–26. http://dx.doi.org/10.1002/vjch.202000078.
Abstract:
AbstractIonic liquids (ILs) have been considered as an alternative class of electrolytes compared to conventional carbonate solvents in rechargeable lithium/sodium batteries. However, the drawbacks of ILs are their reducing ionic conductivity and their large viscosity. Therefore, mixtures of alkyl carbonate solvents with an IL and a sodium bis(trifluoromethane sulfonyl)imide (NaTFSI) have been investigated to develop new electrolytes for sodium‐ion batteries. In this work, N‐Butyl‐N‐methylpyrrolidinium bis(trifluoro‐methanesulfonyl) imide (Py14TFSI) was used as co‐solvent mixing with commercial electrolytes based on the carbonate, i.e. EC‐PC (1:1), EC‐DMC (1:1), and EC‐PC‐DMC (3:1:1). The addition of ionic liquid in the carbonate‐based electrolyte solution results in (i) enhancing ionic conductivity to be comparable with a solvent‐free IL‐based electrolyte, (ii) maintaining the electrochemical stability window, and (iii) IL acted as a retardant rather than a flame‐inhibitor based on the self‐extinguish time (SET) of the mixed electrolyte mixture when exposed to a free flame. All mixed electrolyte systems have been tested in sodium‐coin cells versus Na0.44MnO2 (NMO) and hard carbon (HC) electrodes. The cells show good performances in charge/discharge cycling with a retention > 96 % after 30 cycles (∼90 mAh.g‐1 for NMO and 180 mAh.g‐1 for HC, respectively) demonstrating good interfacial stability and highly stable discharge capacities.
17
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, no. 1 (July 15, 2021): 16–21. http://dx.doi.org/10.3390/oxygen1010003.
Abstract:
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.
18
Huang, Jian-Qiu, Xuyun Guo, Xiuyi Lin, Ye Zhu, and Biao Zhang. "Hybrid Aqueous/Organic Electrolytes Enable the High-Performance Zn-Ion Batteries." Research 2019 (December 2, 2019): 1–10. http://dx.doi.org/10.34133/2019/2635310.
Abstract:
Rechargeable aqueous zinc ion batteries (ZIBs) are considered as one of the most promising systems for large-scale energy storage due to their merits of low cost, environmental friendliness, and high safety. The utilization of aqueous electrolyte also brings about some problems such as low energy density, fast self-discharge, and capacity fading associated with the dissolution of metals in water. To combat the issues, we utilize a freestanding vanadium oxide hydrate/carbon nanotube (V2O5·nH2O/CNT) film as the cathode and probe the performance in aqueous/organic hybrid electrolytes. The corresponding structural and morphological evolution of both V2O5·nH2O/CNT cathode and Zn anode in different electrolytes is explored. The integrity of electrodes and the suppression of zinc dendrites during cycles are largely improved in the hybrid electrolytes. Accordingly, the battery in hybrid electrolyte exhibits high capacities of 549 mAh g-1 at 0.5 A g-1 after 100 cycles and 282 mAh g-1 at 4 A g-1 after 1000 cycles, demonstrating an excellent energy density of 102 Wh kg-1 at a high power of 1500 W kg-1 based on the cathode.
19
Kirchberger, Anna Maria, Patrick Walke, and Tom Nilges. "Effect of Nanostructured Inorganic Ceramic Filler on Poly(ethylene oxide)-Based Solid Polymer Electrolytes." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 991. http://dx.doi.org/10.1149/ma2023-016991mtgabs.
Abstract:
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
20
Rabii, Sanaa, Ayoub Lahmidi, Samir Chtita, Mhammed El Kouali, Mohammed Talbi, and Abdelkbir Errougui. "Molecular dynamics modelling of the structural, dynamic, and dielectric properties of the {LiF - ethylene carbonate} energy storage system at various temperatures." Journal of the Serbian Chemical Society, no. 00 (2024): 61. http://dx.doi.org/10.2298/jsc240205061r.
Abstract:
Lithium-ion batteries (LIBs) play a vital role in advancing the hybrid industry, especially in electric vehicles, as clean and sustainable electrochemical energy sources. However, the prevalent use of organic solvents in the liquid electrolytes of these energy storage systems raises environmental concerns. In this study, we investigated the impact of a polar aprotic solvent, Ethylene Carbonate (EC), on the structural, dynamic, and dielectric properties of the LiF electrolyte using molecular dynamics simulations. By employing the CHARMM 36 force field, our goal was to comprehend the various physicochemical phenomena occurring in this electrolytic system across different temperatures within the saturation region. The structural properties were analyzed through the computation of the radial distribution function (RDF) for various pairs, while the dynamic and dielectric behaviors were elucidated by simulating the self-diffusion coefficient (D) and the dielectric constant (?).
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Mohanty, Debabrata, Shu-Yu Chen, and I.-Ming Hung. "Effect of Lithium Salt Concentration on Materials Characteristics and Electrochemical Performance of Hybrid Inorganic/Polymer Solid Electrolyte for Solid-State Lithium-Ion Batteries." Batteries 8, no. 10 (October 9, 2022): 173. http://dx.doi.org/10.3390/batteries8100173.
Abstract:
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.
22
Zahiri, Beniamin, Chadd Kiggins, Dijo Damien, Michael Caple, Arghya Patra, Carlos Juarez Yescaz, John B. Cook, and Paul V. Braun. "Hybrid Halide Solid Electrolytes and Bottom-up Cell Assembly Enable High Voltage Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 327. http://dx.doi.org/10.1149/ma2022-012327mtgabs.
Abstract:
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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Shah, Rajesh, Vikram Mittal, and Angelina Mae Precilla. "Challenges and Advancements in All-Solid-State Battery Technology for Electric Vehicles." J 7, no. 3 (June 27, 2024): 204–17. http://dx.doi.org/10.3390/j7030012.
Abstract:
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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Spencer Jolly, Dominic, Dominic L. R. Melvin, Isabella D. R. Stephens, Rowena H. Brugge, Shengda D. Pu, Junfu Bu, Ziyang Ning, et al. "Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries." Inorganics 10, no. 5 (April 26, 2022): 60. http://dx.doi.org/10.3390/inorganics10050060.
Abstract:
Hybrid solid-state batteries using a bilayer of ceramic and solid polymer electrolytes may offer advantages over using a single type of solid electrolyte alone. However, the impedance to Li+ transport across interfaces between different electrolytes can be high. It is important to determine the resistance to Li+ transport across these heteroionic interfaces, as well as to understand the underlying causes of these resistances; in particular, whether chemical interphase formation contributes to giving high resistances, as in the case of ceramic/liquid electrolyte interfaces. In this work, two ceramic electrolytes, Li3PS4 (LPS) and Li6.5La3Zr1.5Ta0.5O12 (LLZTO), were interfaced with the solid polymer electrolyte PEO10:LiTFSI and the interfacial resistances were determined by impedance spectroscopy. The LLZTO/polymer interfacial resistance was found to be prohibitively high but, in contrast, a low resistance was observed at the LPS/polymer interface that became negligible at a moderately elevated temperature of 50 °C. Chemical characterization of the two interfaces was carried out, using depth-profiled X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry, to determine whether the interfacial resistance was correlated with the formation of an interphase. Interestingly, no interphase was observed at the higher resistance LLZTO/polymer interface, whereas LPS was observed to react with the polymer electrolyte to form an interphase.
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Spencer Jolly, Dominic, Dominic L. R. Melvin, Isabella D. R. Stephens, Rowena H. Brugge, Shengda D. Pu, Junfu Bu, Ziyang Ning, et al. "Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries." Inorganics 10, no. 5 (April 26, 2022): 60. http://dx.doi.org/10.3390/inorganics10050060.
Abstract:
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, and Henry Michael Woolley. "Hybrid Material Concepts for Thiophosphate-Based Solid-State Batteries." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 984. http://dx.doi.org/10.1149/ma2023-016984mtgabs.
Abstract:
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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Pandurangan, Perumal. "Recent Progression and Opportunities of Polysaccharide Assisted Bio-Electrolyte Membranes for Rechargeable Charge Storage and Conversion Devices." Electrochem 4, no. 2 (April 10, 2023): 212–38. http://dx.doi.org/10.3390/electrochem4020015.
Abstract:
Polysaccharide-based natural polymer electrolyte membranes have had tremendous consideration for the various energy storage operations including wearable electronic and hybrid vehicle industries, due to their unique and predominant qualities. Furthermore, they have fascinating oxygen functionality results of a higher flexible nature and help to form easier coordination of metal ions thus improving the conducting profiles of polymer electrolytes. Mixed operations of the various alkali and alkaline metal–salt-incorporated biopolymer electrolytes based on different polysaccharide materials and their charge transportation mechanisms are detailly explained in the review. Furthermore, recent developments in polysaccharide electrolyte separators and their important electrochemical findings are discussed and highlighted. Notably, the characteristics and ion-conducting mechanisms of different biopolymer electrolytes are reviewed in depth here. Finally, the overall conclusion and mandatory conditions that are required to implement biopolymer electrolytes as a potential candidate for the next generation of clean/green flexible bio-energy devices with enhanced safety; several future perspectives are also discussed and suggested.
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Thangadurai, Venkataraman. "(Invited) Lithium – Sulfur Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 545. http://dx.doi.org/10.1149/ma2022-024545mtgabs.
Abstract:
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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Veelken, Philipp M., Maike Wirtz, Roland Schierholz, Hermann Tempel, Hans Kungl, Rüdiger-A. Eichel, and Florian Hausen. "Investigating the Interface between Ceramic Particles and Polymer Matrix in Hybrid Electrolytes by Electrochemical Strain Microscopy." Nanomaterials 12, no. 4 (February 15, 2022): 654. http://dx.doi.org/10.3390/nano12040654.
Abstract:
The interface between ceramic particles and a polymer matrix in a hybrid electrolyte is studied with high spatial resolution by means of Electrochemical Strain Microscopy (ESM), an Atomic Force Microscope (AFM)-based technique. The electrolyte consists of polyethylene oxide with lithium bis(trifluoromethanesulfonyl)imide (PEO6–LiTFSI) and Li6.5La3Zr1.5Ta0.5O12 (LLZO:Ta). The individual components are differentiated by their respective contact resonance, ESM amplitude and friction signals. The ESM signal shows increased amplitudes and higher contact resonance frequencies on the ceramic particles, while lower amplitudes and lower contact resonance frequencies are present on the bulk polymer phase. The amplitude distribution of the hybrid electrolyte shows a broader distribution in comparison to pure PEO6–LiTFSI. In the direct vicinity of the particles, an interfacial area with enhanced amplitude signals is found. These results are an important contribution to elucidate the influence of the ceramic–polymer interaction on the conductivity of hybrid electrolytes.
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Méry, Adrien, Steeve Rousselot, David Lepage, David Aymé-Perrot, and Mickael Dollé. "Limiting Factors Affecting the Ionic Conductivities of LATP/Polymer Hybrid Electrolytes." Batteries 9, no. 2 (January 28, 2023): 87. http://dx.doi.org/10.3390/batteries9020087.
Abstract:
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.
31
Gerstenberg, Jessica, Dominik Steckermeier, Arno Kwade, and Peter Michalowski. "Effect of Mixing Intensity on Electrochemical Performance of Oxide/Sulfide Composite Electrolytes." Batteries 10, no. 3 (March 7, 2024): 95. http://dx.doi.org/10.3390/batteries10030095.
Abstract:
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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Im, Eunmi, Seok Ju Kang, and Geon Dae Moon. "“Water-in-Salt” and Nasicon Electrolyte-Based Na-CO2 Battery." ECS Meeting Abstracts MA2022-01, no. 4 (July 7, 2022): 537. http://dx.doi.org/10.1149/ma2022-014537mtgabs.
Abstract:
Aprotic electrolytes are much less feasible for producing cost-effective Na metal-based CO2 batteries due to high cost and flammability. As an alternative electrolyte, super-concentrated electrolytes, referred to as “water-in-salt (WiS) electrolytes”, have been received attention due to their wide electrochemical stability window, cost-effectiveness, and non-flammability. However, the highly reactive Na metal prevents the direct use of WiS electrolytes because the unsolvated water molecules would react with the Na Metal. In this study, we demonstrated the ability of a WiS and NASICON electrolyte-based Na-CO2 battery for utilizing CO2 gas and serving as an energy storage cell. The NASICON separator allowed us to fabricate a hybrid Na-CO2 battery comprising Na metal as the anode material and WiS as the cathode electrolyte without damage of Na metal. Additionally, linear sweep voltammetry (LSV) with corresponding differential electrochemical mass spectroscopy (DEMS) measurements rendered the direct observation of H2 evolution retardation with increasing WiS concentration. Furthermore, we introduced a nano-sized Ru catalyst onto the current collector using Joule heating method for reducing the overpotential gap. Consequently, the Na-CO2 batteries with Ru@carbon current collector reduced the overpotential gap and exhibit a cycling endurance of over 75 cycles. Figure 1
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Joraleechanchai, Nattanon, and Montree Sawangphruk. "(Digital Presentation) Free Solvent Molecules in the Electrolyte Leading to Severe Safety Concern of Ni-Rich Li-Ion Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 239. http://dx.doi.org/10.1149/ma2022-012239mtgabs.
Abstract:
The safety of Li-ion batteries is one of the most important factors, if not the most, determining their practical applications. We have found that free carbonate-based solvent molecules in the hybrid electrolyte system can cause severe safety concerns. The 18650 battery cells using the 50% varied-alkyl chain piperidinium-based TFSI result in an immediate and aggressive explosion after applying the impact test (UN38.3) compared with the cell using the conventional electrolyte, having a mild explosion after applying the impact force with 16 s-delayed time. Furthermore, the greater concentration of gases especially C2H4 and CO in the hybrid electrolyte system compared with the conventional electrolyte system was observed by online in situ DEMS, which is evidence for the aggressive explosion of the cell using the hybrid electrolyte. In additionally, the classical MD investigation is suggested that hybrid electrolytes have a high AGG concentration of Li+ and TFSI−, producing a high concentration of the isolated EC or free solvent, which could generate more gases in the fully charged battery cell. Mixing ionic liquids with a carbonate-based solvent as the co-solvent at a fixed salt concentration of 1 M LiPF6 can lead to free carbonate-based molecules causing poor charge storage performance and safety concerns. Keywords: Ni-rich Li-ion bateriesIonic liquids; Safety; Battery explosion; Mismatch electronic properties; 1865 cylindrical cells
34
Walkowiak, Mariusz, Monika Osińska, Teofil Jesionowski, and Katarzyna Siwińska-Stefańska. "Synthesis and characterization of a new hybrid TiO2/SiO2 filler for lithium conducting gel electrolytes." Open Chemistry 8, no. 6 (December 1, 2010): 1311–17. http://dx.doi.org/10.2478/s11532-010-0110-3.
Abstract:
AbstractThis paper describes the synthesis and properties of a new type of ceramic fillers for composite polymer gel electrolytes. Hybrid TiO2-SiO2 ceramic powders have been obtained by co-precipitation from titanium(IV) sulfate solution using sodium silicate as the precipitating agent. The resulting submicron-size powders have been applied as fillers for composite polymer gel electrolytes for Li-ion batteries based on poly(vinylidene fluoride-co-hexafluoropropylene) (PVdF/HFP) copolymeric membranes. The powders, dry membranes and gel electrolytes have been examined structurally and electrochemically, showing favorable properties in terms of electrolyte uptake and electrochemical characteristics in Li-ion cells.
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Ryu, Kun, Kyungbin Lee, Hyun Ju, Jinho Park, Ilan Stern, and Seung Woo Lee. "Ceramic/Polymer Hybrid Electrolyte with Enhanced Interfacial Contact for All-Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2621. http://dx.doi.org/10.1149/ma2022-0272621mtgabs.
Abstract:
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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Mroziewicz, Aleksandra A., Karolina Solska, Grażyna Zofia Żukowska, and Magdalena Skunik-Nuckowska. "Water/N,N-Dimethylacetamide-Based Hybrid Electrolyte and Its Application to Enhanced Voltage Electrochemical Capacitors." Batteries 10, no. 6 (June 19, 2024): 213. http://dx.doi.org/10.3390/batteries10060213.
Abstract:
The growing interest in hybrid (aqueous–organic) electrolytes for electrochemical energy storage is due to their wide stability window, improved safety, and ease of assembly that does not require a moisture-free atmosphere. When it comes to applications in electrochemical capacitors, hybrid electrolytes are expected to fill the gap between high-voltage organic systems and their high discharge rate aqueous counterparts. This article discusses the potential applicability of aqueous–organic electrolytes utilizing water/N,N-dimethylacetamide (DMAc) solvent mixture, and sodium perchlorate as a source of charge carriers. The hydrogen bond formation between H2O and DMAc (mole fraction xDMAc = 0.16) is shown to regulate the original water and cation solvation structure, thus reducing the electrochemical activity of the primary aqueous solution both in the hydrogen (HER) and oxygen (OER) evolution reactions region. As a result, an electrochemical stability window of 3.0 V can be achieved on titanium electrodes while providing reasonable ionic conductivity of 39 mS cm−1 along with the electrolyte’s flame retardant and anti-freezing properties. Based on the diagnostic electrochemical studies, the operation conditions for carbon/carbon capacitors have been carefully optimized to adjust the potential ranges of the individual electrodes to the electrochemical stability region. The system with the appropriate electrode mass ratio (m+/m− = 1.51) was characterized by a wide operating voltage of 2.0 V, gravimetric energy of 13.2 Wh kg−1, and practically a 100% capacitance retention after 10,000 charge–discharge cycles. This translates to a significant rise in the maximum energy of 76% when compared to the aqueous counterpart. Additionally, reasonable charge–discharge rates and anti-freeze properties of the developed electrolyte enable application in a broad temperature range down to −20 °C, which is demonstrated as well.
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Zhu, Jun-Jie, Luis Martinez-Soria, and Pedro Gomez-Romero. "Coherent Integration of Organic Gel Polymer Electrolyte and Ambipolar Polyoxometalate Hybrid Nanocomposite Electrode in a Compact High-Performance Supercapacitor." Nanomaterials 12, no. 3 (February 1, 2022): 514. http://dx.doi.org/10.3390/nano12030514.
Abstract:
We report a gel polymer electrolyte (GPE) supercapacitor concept with improved pathways for ion transport, thanks to a facile creation of a coherent continuous distribution of the electrolyte throughout the electrode. Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) was chosen as the polymer framework for organic electrolytes. A permeating distribution of the GPE into the electrodes, acting both as integrated electrolyte and binder, as well as thin separator, promotes ion diffusion and increases the active electrode–electrolyte interface, which leads to improvements both in capacitance and rate capability. An activation process induced during the first charge–discharge cycles was detected, after which, the charge transfer resistance and Warburg impedance decrease. We found that a GPE thickness of 12 μm led to optimal capacitance and rate capability. A novel hybrid nanocomposite material, formed by the tetraethylammonium salt of the 1 nm-sized phosphomolybdate cluster and activated carbon (AC/TEAPMo12), was shown to improve its capacitive performance with this gel electrolyte arrangement. Due to the homogeneous dispersion of PMo12 clusters, its energy storage process is non-diffusion-controlled. In the symmetric capacitors, the hybrid nanocomposite material can perform redox reactions in both the positive and the negative electrodes in an ambipolar mode. The volumetric capacitance of a symmetric supercapacitor made with the hybrid electrodes increased by 40% compared to a cell with parent AC electrodes. Due to the synergy between permeating GPE and the hybrid electrodes, the GPE hybrid symmetric capacitor delivers three times more energy density at higher power densities and equivalent cycle stability compared with conventional AC symmetric capacitors.
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Proffit, Danielle L., Albert L. Lipson, Baofei Pan, Sang-Don Han, Timothy T. Fister, Zhenxing Feng, Brian J. Ingram, Anthony K. Burrell, and John T. Vaughey. "Reducing Side Reactions Using PF6-based Electrolytes in Multivalent Hybrid Cells." MRS Proceedings 1773 (2015): 27–32. http://dx.doi.org/10.1557/opl.2015.590.
Abstract:
ABSTRACTThe need for higher energy density batteries has spawned recent renewed interest in alternatives to lithium ion batteries, including multivalent chemistries that theoretically can provide twice the volumetric capacity if two electrons can be transferred per intercalating ion. Initial investigations of these chemistries have been limited to date by the lack of understanding of the compatibility between intercalation electrode materials, electrolytes, and current collectors. This work describes the utilization of hybrid cells to evaluate multivalent cathodes, consisting of high surface area carbon anodes and multivalent nonaqueous electrolytes that are compatible with oxide intercalation electrodes. In particular, electrolyte and current collector compatibility was investigated, and it was found that the carbon and active material play an important role in determining the compatibility of PF6-based multivalent electrolytes with carbon-based current collectors. Through the exploration of electrolytes that are compatible with the cathode, new cell chemistries and configurations can be developed, including a magnesium-ion battery with two intercalation host electrodes, which may expand the known Mg-based systems beyond the present state of the art sulfide-based cathodes with organohalide-magnesium based electrolytes.
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Zhang, L. X., Y. Z. Li, L. W. Shi, R. J. Yao, S. S. Xia, Y. Wang, and Y. P. Yang. "Electrospun Polyethylene Oxide (PEO)-Based Composite polymeric nanofiber electrolyte for Li-Metal Battery." Journal of Physics: Conference Series 2353, no. 1 (October 1, 2022): 012004. http://dx.doi.org/10.1088/1742-6596/2353/1/012004.
Abstract:
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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Chikkatti, Bipin S., Ashok M. Sajjan, Prakash B. Kalahal, Nagaraj R. Banapurmath, T. M. Yunus Khan, Shaik Dawood Abdul Khadar, Shaik Mohamed Shamsudeen, and A. B. Raju. "A Novel Poly(vinyl alcohol)–tetraethylorthosilicate Hybrid Gel Electrolyte for Lead Storage Battery." Gels 8, no. 12 (December 2, 2022): 791. http://dx.doi.org/10.3390/gels8120791.
Abstract:
The gel electrolyte significantly influences gel valve-regulated lead acid battery performance. To address this, the paper describes the preparation of novel polymer gel electrolytes using poly (vinyl alcohol) (PVA) and tetraethylorthosilicate (TEOS) for valve-regulated lead–acid batteries. FTIR technique is used to confirm the chemical reaction between PVA and TEOS. Electrochemical analyses such as cyclic voltammetry and electrochemical impedance spectroscopy were applied to optimize the concentration of PVA-TEOS polymer gel electrolyte. The optimum concentration of polymer gel electrolyte was determined as 20 wt% of TEOS in PVA (PE-1) with higher anodic peak and lower Rs and Rct values. The Galvanostatic charge–discharge tests were performed on the optimized gel system prototype battery. The highest capacity of 6.86 × 10−5 Ah at a current density of 0.2 mA cm−2 was achieved with an excellent capacity retention ratio of 85.7% over 500 cycles. The exceptional cycle performance and high capacity make PVA-TEOS gel electrolyte a promising candidate for practical battery application.
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Lan, Pei-Ling, I.-Chih Ni, Chih-I. Wu, Cheng-Che Hsu, I.-Chun Cheng, and Jian-Zhang Chen. "Ultrafast Fabrication of H2SO4, LiCl, and Li2SO4 Gel Electrolyte Supercapacitors with Reduced Graphene Oxide (rGO)-LiMnOx Electrodes Processed Using Atmospheric-Pressure Plasma Jet." Micromachines 14, no. 9 (August 30, 2023): 1701. http://dx.doi.org/10.3390/mi14091701.
Abstract:
Pastes containing reduced graphene oxide (rGO) and LiCl-Mn(NO3)2·4H2O are screen-printed on a carbon cloth substrate and then calcined using a nitrogen atmospheric-pressure plasma jet (APPJ) for conversion into rGO-LiMnOx nanocomposites. The APPJ processing time is within 300 s. RGO-LiMnOx on carbon cloth is used to sandwich H2SO4, LiCl, or Li2SO4 gel electrolytes to form hybrid supercapacitors (HSCs). The areal capacitance, energy density, and cycling stability of the HSCs are evaluated using electrochemical measurement. The HSC utilizing the Li2SO4 gel electrolyte exhibits enhanced electrode–electrolyte interface reactions and increased effective surface area due to its high pseudocapacitance (PC) ratio and lithium ion migration rate. As a result, it demonstrates the highest areal capacitance and energy density. The coupling of charges generated by embedded lithium ions with the electric double-layer capacitance (EDLC) further contributed to the significant overall capacitance enhancement. Conversely, the HSC with the H2SO4 gel electrolyte exhibits better cycling stability. Our findings shed light on the interplay between gel electrolytes and electrode materials, offering insights into the design and optimization of high-performance HSCs.
42
Tian, Lanlan, Lian Xiong, Xuefang Chen, Haijun Guo, Hairong Zhang, and Xinde Chen. "Enhanced Electrochemical Properties of Gel Polymer Electrolyte with Hybrid Copolymer of Organic Palygorskite and Methyl Methacrylate." Materials 11, no. 10 (September 24, 2018): 1814. http://dx.doi.org/10.3390/ma11101814.
Abstract:
Gel polymer electrolyte (GPE) is widely considered as a promising safe lithium-ion battery material compared to conventional organic liquid electrolyte, which is linked to a greater risk of corrosive liquid leakage, spontaneous combustion, and explosion. GPE contains polymers, lithium salts, and liquid electrolyte, and inorganic nanoparticles are often used as fillers to improve electrochemical performance. However, such composite polymer electrolytes are usually prepared by means of blending, which can impact on the compatibility between the polymer and filler. In this study, the hybrid copolymer poly (organic palygorskite-co-methyl methacrylate) (poly(OPal-MMA)) is synthesized using organic palygorskite (OPal) and MMA as raw materials. The poly(OPal-MMA) gel electrolyte exhibits an ionic conductivity of 2.94 × 10−3 S/cm at 30 °C. The Li/poly(OPal-MMA) electrolyte/LiFePO4 cell shows a wide electrochemical window (approximately 4.7 V), high discharge capacity (146.36 mAh/g), and a low capacity-decay rate (0.02%/cycle).
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Giffin, Guinevere A., Mara Goettlinger, Hendrik Bohn, Simone Peters, Mario Weller, Alexander Naßmacher, Timo Brändel, and Alex Friesen. "Development of a Polymer-Based Silicon-NMC Solid-State Cell." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 373. http://dx.doi.org/10.1149/ma2023-022373mtgabs.
Abstract:
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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Shah, Vaidik, and Yong Lak Joo. "Rationally Designed in-Situ Gelled Polymer-Ceramic Hybrid Electrolyte Enables Superior Performance and Stability in Quasi-Solid-State Lithium-Sulfur Batteries." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 535. http://dx.doi.org/10.1149/ma2023-024535mtgabs.
Abstract:
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.
45
Thangadurai, Venkataraman. "(Invited) Garnet Solid Electrolytes for Advanced All-Solid-State Li Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 47 (October 9, 2022): 1759. http://dx.doi.org/10.1149/ma2022-02471759mtgabs.
Abstract:
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.
46
Zhai, Yanfang, Wangshu Hou, Zongyuan Chen, Zhong Zeng, Yongmin Wu, Wensheng Tian, Xiao Liang, et al. "A hybrid solid electrolyte for high-energy solid-state sodium metal batteries." Applied Physics Letters 120, no. 25 (June 20, 2022): 253902. http://dx.doi.org/10.1063/5.0095923.
Abstract:
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.
47
Tsai, Hsin-Yen, Munusamy Sathish Kumar, Balaraman Vedhanarayanan, Hsin-Hui Shen, and Tsung-Wu Lin. "Urea-Based Deep Eutectic Solvent with Magnesium/Lithium Dual Ions as an Aqueous Electrolyte for High-Performance Battery-Supercapacitor Hybrid Devices." Batteries 9, no. 2 (January 18, 2023): 69. http://dx.doi.org/10.3390/batteries9020069.
Abstract:
A new deep eutectic solvent (DES) made from urea, magnesium chloride, lithium perchlorate and water has been developed as the electrolyte for battery-supercapacitor hybrid devices. The physicochemical characteristics of DES electrolytes and potential interactions between electrolyte components are well analyzed through electrochemical and spectroscopic techniques. It has been discovered that the properties of DES electrolytes are highly dependent on the component ratio, which allows us to engineer the electrolyte to meet the requirement of the battery application. Perylene tetracarboxylic di-imide and reduced graphene oxide ha ve been combined to produce a composite (PTCDI/rGO) that has been tested as the anode in DES electrolyte. This composite shows that the capacitive contribution is greater than 90% in a low scan rate, resulting in the high rate capability. The PTCDI/rGO electrode exhibits no sign of capacity degradation and its coulombic efficiency is close to 99% after 200 cycles, which suggests excellent reversibility and stability. On the other hand, the electrochemical performance of lithium manganese oxide as the cathode material is studied in DES electrolyte, which exhibits the maximum capacity of 76.5 mAh/g at 0.03 A/g current density. After being successfully examined in terms of electrode kinetics, capacity performance, and rate capability, the anode and cathode materials are combined to construct a two-electrode system with DES electrolyte. At a current density of 0.03 A/g, this system offers 43.5 mAh/g specific capacity and displays 55.5% retention of the maximum capacity at 1 A/g. Furthermore, an energy density of 53 Wh/kg is delivered at a power density of 35 W/kg.
48
Yan, Shuo, Chae-Ho Yim, Ali Merati, Elena A. Baranova, Yaser Abu-Lebdeh, and Arnaud Weck. "Interfacial Challenge for Solid-State Lithium Batteries- Liquid Addition." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 1010. http://dx.doi.org/10.1149/ma2023-0161010mtgabs.
Abstract:
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.
49
Gálvez, Francisco, Marta Cabello, Pedro Lavela, Gregorio F. Ortiz, and José L. Tirado. "Sustainable and Environmentally Friendly Na and Mg Aqueous Hybrid Batteries Using Na and K Birnessites." Molecules 25, no. 4 (February 19, 2020): 924. http://dx.doi.org/10.3390/molecules25040924.
Abstract:
Sodium and magnesium batteries with intercalation electrodes are currently alternatives of great interest to lithium in stationary applications, such as distribution networks or renewable energies. Hydrated laminar oxides such as birnessites are an attractive cathode material for these batteries. Sodium and potassium birnessite samples have been synthesized by thermal and hydrothermal oxidation methods. Hybrid electrochemical cells have been built using potassium birnessite in aqueous sodium electrolyte, when starting in discharge and with a capacity slightly higher than 70 mA h g−1. Hydrothermal synthesis generally shows slightly poorer electrochemical behavior than their thermal counterparts in both sodium and potassium batteries. The study on hybrid electrolytes has resulted in the successful galvanostatic cycling of both sodium birnessite and potassium birnessite in aqueous magnesium electrolyte, with maximum capacities of 85 and 50 mA h g−1, respectively.
50
Lu, Xuejun, María C. Gutiérrez, M. Luisa Ferrer, Xuejun Lu, and Jian Liu. "“Tri-Solvent-in-Salt” Electrolytes for High-Performance Supercapacitors." ECS Meeting Abstracts MA2022-01, no. 35 (July 7, 2022): 1412. http://dx.doi.org/10.1149/ma2022-01351412mtgabs.
Abstract:
Electrolytes chemistry for high-performance supercapacitors (SCs) has been addressed recently, where solvents included in electrolyte composition dissolving or mixing the electrochemically active salts or ILs have been typically seen as a mere medium.[1] Specifically, attention regarding the achievement of high-performacne SCs has also been paid to, e.g., water-in-salt (WIS), solvent-in-salt (SIS), and bi-solvent-in-salt (BSIS) electrolytes, demonstrating that solvent molecules may indeed play a more active role.[2 - 4] In this presentation, we will talk about the design of a tri-solvent-in-salt (TSIS) electrolyte where every solvent contributed (with an IL, i.e., EMIMBF4) to the formation of an electrochemically active hydrogen bond (HB) complex structure. Raman and NMR spectroscopies, as well as molecular dynamic (MD) simulations, helped elucidate the ratio among all compounds (e.g., solvents and IL) in the HB complex structure that best works as an electrolyte. For instance, the eutectic mixture of H2O and dimethylsulfoxide (DMSO) in a 2 to 1 molar ratio primary HB complex structures with mixed EMIMBF4 offers a low melting point and low flammability, then add acetonitrile (CH3CN) in different molar ratios providing an improvement of the rate capability to the resulting electrolyte. As compared to other electrolytes, the TSIS electrolyte composed in a molality of 5.8 m (TSIS-5.8) showed the cost efficiency and exhibited a low self-extinction rate. Moreover, SCs operating with TSIS-5.8, at -70 °C and up to 2.7 V provided energy densities of ca. 49 and 18 Wh kg-1, respectively, power densities of 10,000 and 17,000 W kg-1, the capacitance retention of ca. 82% after 15,000 cycles at 4 A g-1 and a self-discharge as low as 22%. The use of ternary solvent mixtures combining different solvents in the proper molar ratios opens up an easy and low-cost path to design many new electrolytes in terms of non-flammability, non-toxicity, high electrical conductivity, and wide electrochemical stability window (ESW). Forthcoming research could use the knowledge provided by this work in terms of ions solvation and transport in TSIS electrolytes and explore the interfacial interactions between electrolyte and electrode material to determine their respective relevance in the performance of SCs. Keywords: tri-solvent-in-salt (TSIS), hydrogen bond, eutectic mixtures, supercapacitors Reference ： [1] F. Béguin, et al. Carbons and electrolytes for advanced supercapacitors. Adv. Mater., 26 (2014), 2219-2251. [2] Q. Dou, et al. Safe and high-rate supercapacitors based on an ‘‘Acetonitrile/Water in Salt’’ hybrid electrolyte. Energy Environ. Sci, 11 (2018), 3212-3219. [3] X. Lu, et al. Aqueous-Eutectic-in-Salt Electrolytes for High-Energy-Density Supercapacitors with an Operational Temperature Window of 100 °C, from −35 to +65 °C. ACS Appl. Mater. Interfaces 2020, 12, 26, 29181–29193. [4] X. Lu, et al. Aqueous Co-Solvent in Zwitterionic-based Protic Ionic Liquids as Electrolytes in 2.0 V Supercapacitors. ChemSusChem 2020, 13, 5983. [5] X. Lu, et al. EMIMBF4 in ternary liquid mixtures of water, dimethyl sulfoxide and acetonitrile as “tri-solvent-in-salt” electrolytes for high-performance supercapacitors operating at -70 °C. Energy Storage Mater., 40, (2021), 368-385.