期刊
NANO LETTERS
卷 17, 期 11, 页码 6974-6982出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b03498
关键词
Li-ion battery; space-charge layer; thin-film; pulsed laser deposition; solid electrolyte; XPS
类别
资金
- Laboratory Directed Research and Development (LDRD) Program at Sandia National Laboratories
- U.S. Department of Energy's National Nuclear Security Administration [DE-NA-0003525]
- Science of Precision Multifunctional Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DESC0001160]
Efficient and reversible charge transfer is essential to realizing high-performance solid-state batteries. Efforts to enhance charge transfer at critical electrode-electrolyte interfaces have proven successful, yet interfacial chemistry and its impact on cell function remains poorly understood. Using X-ray photoelectron spectroscopy combined with electrochemical techniques, we elucidate chemical coordination near the LiCoO2-LIPON interface, providing experimental validation of space-charge separation. Space-charge layers, defined by local enrichment and depletion of charges, have previously been theorized and modeled, but the unique chemistry of solid-state battery interfaces is now revealed. Here we highlight the non-Faradaic migration of Li+ ions from the electrode to the electrolyte, which reduces reversible cathodic capacity by similar to 15%. Inserting a thin, ion-conducting LiNbO3 interlayer between the electrode and electrolyte, however, can reduce space-charge separation, mitigate the loss of Li+ from LiCoO2, and return cathodic capacity to its theoretical value. This work illustrates the importance of interfacial chemistry in understanding and improving solid-state batteries.
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