Journal
ADVANCED MATERIALS
Volume 34, Issue 8, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202108400
Keywords
carbonate electrolytes; lithium-metal batteries; solid electrolyte interface; solvation structure
Categories
Funding
- National Key Research and Development Program of China [2021YFB2500051, 2019YFA0705700]
- National Natural Science Foundation of China [52072205]
- Start-up Funds of Tsinghua Shenzhen International Graduate School and Shenzhen Geim Graphene Center
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By adding lithium nitrate additive and a small amount of tetramethylurea as a multifunctional cosolvent to a commercial carbonate electrolyte, it is possible to improve the performance and cycle life of lithium-metal batteries, providing a simple and effective way to extend the use of commercial carbonate electrolytes for next-generation battery systems.
Lithium-metal batteries (LMBs) are considered as promising next-generation batteries due to their high energy density. However, commercial carbonate electrolytes cannot be used in LMBs due to their poor compatibility with the lithium-metal anode and detrimental hydrogen fluoride (HF) generation by lithium hexafluorophosphate decomposition. By introducing lithium nitrate additive and a small amount of tetramethylurea as a multifunctional cosolvent to a commercial carbonate electrolyte, NO3-, which is usually insoluble, can be introduced into the solvation structure of Li+ to form a conductive and stable solid electrolyte interface. At the same time, HF generation is suppressed by manipulating the solvation structure and a scavenging effect. As a result, the Coulombic efficiency (CE) of Li||Cu half cells using the designed carbonate electrolyte can reach 98.19% at room temperature and 96.14% at low temperature (-15 degrees C), and Li||LiFePO4 cells deliver a high capacity retention of 94.9% with a high CE of 99.6% after 550 cycles. This work provides a simple and effective way to extend the use of commercial carbonate electrolytes for next-generation battery systems.
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