Regulating Non-Equilibrium Solvation Structure in Locally Concentrated Ionic Liquid Electrolytes for Wide-Temperature and High-Voltage Lithium Metal Batteries.

Autor: Tu H; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Wang Z; Institute of Physics Chinese Academy of Sciences, Beijing Advanced Innovation Center for Materials Genome Engineering Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and Devices, CHINA., Xue J; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Tang Z; University of Science and Technology of China, i-lab, Suzhou, CHINA., Liu Y; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Liu X; Jiangxi Science and Technology Normal University, Jiangxi Key Laboratory of Flexible Electronics, CHINA., Liu L; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Lu S; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Weng S; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Gao Y; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Sun G; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Liu Z; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Peng K; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Zhang X; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Li D; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Wu G; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA., Liu M; Guangxi University, Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, School of Resources, Environment and Materials, CHINA., Hu J; Soochow University, National Engineering Laboratory for Modern Silk College of Textile and Clothing Engineering Research Center of Cooperative Innovation for Functional Organic/ Polymer Material Micro/Nanofabrication, CHINA., Li H; Chinese Academy of Sciences Institute of Physics, Beijing Advanced Innovation Center for Materials Genome Engineering Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and Devices, CHINA., Xu J; SINANO: Suzhou Institute of Nano-tech and Nano-bionics, No. 398 Ruoshui Road, SEID, Suzhou Industrial Park, Suzhou, CHINA., Wu X; Suzhou Institute of Nano-tech and Nano-bionics, i-lab, CHINA.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Oct 04, pp. e202412896. Date of Electronic Publication: 2024 Oct 04.
DOI: 10.1002/anie.202412896
Abstrakt: The development of high-voltage lithium metal batteries (LMBs) encounters significant challenges due to aggressive electrode chemistry. Recently, locally concentrated ionic liquid electrolytes (LCILEs) have garnered attention for their exceptional stability with both Li anodes and high-voltage cathodes. However, there remains a limited understanding of how diluents in LCILEs affect the thermodynamic stability of the solvation structure and transportation dynamics of Li+ ions. Herein, we propose a wide-temperature LCILEs with 1,3-dichloropropane (DCP13) diluent to construct a non-equilibrium solvation structure under external electric field, wherein the DCP13 diluent enters the Li+ ion solvation sheath to enhance Li+ ion transport and suppress oxidative side reactions at high-nickel cathode (LiNi0.9Co0.05Mn0.05O2, NCM90).Consequently, a Li/NCM90 cell utilizing this LCILE achieves a high capacity retention of 94% after 240 cycles at 4.3 V, also operates stably at high cut-off voltages from 4.4 to 4.6 V and over a wide temperature range from -20 to 60 °C. Additionally, an Ah-level pouch cell with this LCILE simultaneously achieves high-energy-density and stable cycling, manifesting the practical feasibility. This work redefines the role of diluents in LCILEs, providing inspiration for electrolyte design in developing high-energy-density batteries.
(© 2024 Wiley‐VCH GmbH.)
Databáze: MEDLINE