Article
Chemistry, Physical
Thuy Duong Pham, Abdullah Bin Faheem, So Yeon Chun, Jung-Rae Rho, Kyungwon Kwak, Kyung-Koo Lee
Summary: This study shows the potential for enhancing the performance of lithium metal batteries (LMBs) by modulating the ion solvation structures in the electrolyte through mixing different salts. A highly promising electrolyte system with improved conductivity, Coulombic efficiency, and stability of solid-electrolyte interface layer is proposed, offering a new avenue towards commercial LMBs.
ADVANCED ENERGY MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Xu Liu, Alessandro Mariani, Henry Adenusi, Stefano Passerini
Summary: Non-flammable ionic liquid electrolytes (ILEs) are potential candidates for safer and longer-lasting lithium metal batteries (LMBs), but their high viscosity and inadequate Li+ transport restrict their practical use. Recently, diluting ILEs with non-solvating and low-viscosity co-solvents has been employed to overcome these challenges. The resulting locally concentrated ionic liquid electrolytes (LCILEs) exhibit lower viscosity, faster Li+ transport, and improved compatibility with lithium metal anodes, making them promising options for next-generation high-energy-density LMBs. This article provides a summary of the progress made in the development of LCILEs, including their physicochemical properties, solution structures, and applications in LMBs with various high-energy cathode materials. Furthermore, future research directions for LCILEs are outlined to enhance our understanding and achieve better cell performance.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xu Liu, Alessandro Mariani, Thomas Diemant, Xu Dong, Po-Hua Su, Stefano Passerini
Summary: A new electrolyte for low-temperature lithium metal batteries is proposed, which shows good performance in sub-zero conditions. By using this electrolyte, dendrite-free operation of lithium metal anodes at -20℃ and 0.5 mA cm(-2) with a Coulombic efficiency of 98.9% is achieved.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Zhipeng Jiang, Tao Yang, Chen Li, Jiahang Zou, Hanxu Yang, Qingan Zhang, Yongtao Li
Summary: This article proposes a new strategy for designing ether-based electrolytes to achieve stability in high-voltage lithium metal batteries. By co-adding LiNO3 and vinylene carbonate (VC), a unique organic-inorganic bilayer interfacial protective layer is formed, which effectively suppresses electrolyte side reactions and enhances electrode stability, resulting in optimized ether-based electrolytes with high Li-ion conductivity and high-voltage stability.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Xu Liu, Thomas Diemant, Alessandro Mariani, Xu Dong, Maria Enrica Di Pietro, Andrea Mele, Stefano Passerini
Summary: This article proposes a new low-flammability locally concentrated ionic liquid electrolyte (LCILE) for Li/sulfurized polyacrylonitrile (SPAN) batteries. The LCILE forms stable electrolyte/electrode interfaces on both the lithium-metal anodes (LMAs) and SPAN cathodes, leading to improved battery performance and cycling stability.
ADVANCED MATERIALS
(2022)
Article
Engineering, Environmental
Zhu Liao, Anyi Hu, Chenxi Huang, Enyou Zhao, Akihiro Orit, Zhengxi Zhang, Li Yang
Summary: In this study, a plastic crystal electrolyte (APCE) with high concentration of anions was developed, ensuring good stability and advantages of concentrated electrolytes. The deformable property of the electrolyte allows for excellent physical contact with electrodes. Solid-state batteries using APCE exhibited superior long-cycling performance and excellent flexibility. The electrolyte also passed harsh penetration tests and showed high energy density, indicating its potential for next-generation solid-state batteries.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Chongyang Liu, Shi Wang, Xinyi Wu, Shijun Xiao, Chao Liu, Henan Cai, Wen-Yong Lai
Summary: Inspired by the unique mesh geometry of fishing nets and knotted fiber structures, new crosslinkers and elastic components are introduced into polyzwitterionic electrolytes to construct high-strength and ultra-flexible fishing-net-like structure electrolytes. The crosslinkers rich in -NH form chemical and physical crosslinking points, resulting in high strength, while the elastic segments provide super flexibility. The collective regulation of anions and Li+ by the polymer backbone enables stable Li+ deposition and suppresses the growth of lithium dendrites. This work presents a new perspective for constructing polymer electrolytes with synergistic cation-anion regulation functions for high safety and high energy density solid-state lithium batteries.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Xu Liu, Alessandro Mariani, Maider Zarrabeitia, Maria Enrica Di Pietro, Xu Dong, Giuseppe Antonio Elia, Andrea Mele, Stefano Passerini
Summary: Organic cations significantly influence the electrochemical performance of lithium metal batteries by affecting the coordination of FSI- and the formation of solid-electrolyte interphase (SEI). Two different LCILEs with organic cations Pyr(14)(+) and Emim(+) show differences in viscosity, Li+ transport rate, and lithium plating/stripping efficiency, resulting in improved capacity and retention in Li/EmiBE/LiNi0.8Mn0.1Co0.1O2 cells compared to PyrBE-based cells.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Xu Liu, Alessandro Mariani, Thomas Diemant, Maria Enrica Di Pietro, Xu Dong, Andrea Mele, Stefano Passerini
Summary: Trifluoromethoxybenzene as a cosolvent in locally concentrated ionic liquid electrolytes (LCILEs) can enhance the protective electrode/electrolyte interphases (EEIs) in lithium metal batteries, leading to stable cycling of the batteries.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Dengji Xiao, Qian Li, Dan Luo, Rui Gao, Zhaoqiang Li, Ming Feng, Tyler Or, Lingling Shui, Guofu Zhou, Xin Wang, Zhongwei Chen
Summary: This study reveals that the unstable solid electrolyte interface (SEI) in Li metal batteries (LMBs) mainly originates from the kinetic instability of Li+-solvation structures in the electrolyte. By integrating preferentially adsorbed anions into the Li+-solvation structures, the formation of an anion-derived SEI layer with high Li-ion conductivity and low Li atom adhesion energy is achieved, facilitating high Coulombic efficiency and stable cycling in realistic testing conditions.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Physical
Zhicheng Wang, Fengrui Zhang, Yiyang Sun, Lei Zheng, Yanbin Shen, Daosong Fu, Wanfei Li, Anran Pan, Lei Wang, Jingjing Xu, Jianchen Hu, Xiaodong Wu
Summary: An intrinsically nonflammable ionic liquid-based localized highly concentrated electrolyte (LHCE) has been designed, which significantly improves the performance of Li-metal batteries (LMBs) by enhancing ionic conductivity and suppressing Li dendrite growth. The LHCE exhibits high Coulombic efficiency and stable cycling performance over thousands of cycles, making it suitable for various LMB systems. This electrolyte shows great potential for practical application in high-performance batteries.
ADVANCED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Maria Martinez-Ibanez, Nicola Boaretto, Alexander Santiago, Leire Meabe, Xiaoen Wang, Oihane Zugazua, Inigo Raposo, Maria Forsyth, Michel Armand, Heng Zhang
Summary: This paper reports a highly-concentrated FSI-based ternary gel polymer electrolyte (TGPE) with high lithium-ion conductivities, wide electrochemical stability, and superior compatibility with lithium metal electrode. The TGPE enables stable Li plating and stripping processes, as well as high discharge capacity of a Li||Li(Ni0.6Mn0.2Co0.2)O2 cell at ambient temperatures. This study not only provides safe and highly conductive polymer electrolytes but also enhances our understanding of the role of FSI anions in high-energy lithium metal batteries.
JOURNAL OF POWER SOURCES
(2023)
Article
Engineering, Chemical
Honghao Yang, Junyi Ji, Hongjiao Li, Bin Liang
Summary: Salt-concentrated nonaqueous electrolytes have gained significant attention for their ability to increase battery stability through the formation of anion-derived solid electrolyte interphases (SEIs). However, the relationship between their microscopic solvation structures and electrolyte performance, particularly Li-ion conductivity, remains unclear. In this study, we used ab initio molecular dynamics simulations and density functional theory calculations to examine three designed electrolytes: lithium bis(fluorosulfonyl)imide (LiFSI) with acetonitrile (AN), 1,2-dimethoxyethane (DME), and 2,2-dimethyl-3,6,9-trioxa-2-siladecane (siloxane). Our results showed that Li-ion conduction occurs when the solvation structure changes within a few tens of fs, involving the binding and debinding of solvent and FSI anion with the Li-center. The dynamics of solvent-Li binding decreased with an increase in solvation sheath strength, influenced by solvent polarity. In the siloxane-LiFSI system, a steric shielding effect was observed, resulting in nonconductive behavior at a concentration of 3 mol L-1. Despite the high concentration of each electrolyte (>= 5 mol L-1), a certain amount of free solvents remained according to the simulation results. Our findings contribute to a better understanding of Li-ion conduction in salt-concentrated electrolytes and provide insights for designing high-performance electrolytes.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Physical
Xu Liu, Alessandro Mariani, Thomas Diemant, Maria Enrica Di Pietro, Xu Dong, Matthias Kuenzel, Andrea Mele, Stefano Passerini
Summary: A locally concentrated ionic liquid electrolyte (LCILE) was developed by adding dFBn as a cosolvent, which improves the cycling performance and stability of lithium metal batteries.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Shuang-Jie Tan, Wen-Peng Wang, Yi-Fan Tian, Sen Xin, Yu-Guo Guo
Summary: This article summarizes the challenges of electrolytes in rechargeable Li-metal batteries (RLBs) and proposes requirements for improving battery performance. It also reviews the achievements of liquid- and solid-state electrolytes in RLBs, analyzes their drawbacks, and offers solutions. The article outlines the development strategy of in situ gelation electrolytes and calls for more attention to battery safety research in pouch cell users.
ADVANCED FUNCTIONAL MATERIALS
(2021)
