Nonsacrificial Additive for Tuning the Cathode–Electrolyte Interphase of Lithium-Ion Batteries

Zou, Lianfeng; Gao, Peiyuan; Jia, Haiping; Cao, Xia; Wu, Haiping; Wang, Hui; Zhao, Wengao; Matthews, Bethany E.; Xu, Zhijie; Li, Xiaolin; Zhang, Ji-Guang; Xu, Wu; Wang, Chongmin

doi:10.1021/acsami.1c20789

Nonsacrificial Additive for Tuning the Cathode–Electrolyte Interphase of Lithium-Ion Batteries

Journal Article · Mon Jan 10 19:00:00 EST 2022 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c20789· OSTI ID:2569970

Zou, Lianfeng ^[1]; ^[1]; Jia, Haiping ^[1]; Cao, Xia ^[1]; Wu, Haiping ^[1]; Wang, Hui ^[1]; Zhao, Wengao ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; Xu, Wu ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Solid–electrolyte interphases is essential for stable cycling of rechargeable batteries. The traditional approach for interphase design follows the decomposition of additives prior to the host electrolyte, which, as governed by the thermodynamic rule, however, inherently limits the viable additives. Here we report an alternative approach of using a nonsacrificial additive. This is exemplified by the localized high-concentration electrolytes, where the fluoroethylene carbonate (FEC) plays a nonsacrificial role for modifying the chemistry, structure, and formation mechanism of the cathode–electrolyte interphase (CEI) layers toward enhanced cycling stability. On the basis of ab initio molecular dynamics simulations, we further reveal that the unexpected activation of the otherwise inert species in the interphase formation is due to the FEC–Li⁺ coordinated environment that altered the electronic states of reactants. In conclusion, the nonsacrificial additive on CEI formation opens up alternative avenues for the interphase design through the use of the commonly overlooked, anodically stable compounds.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2569970

Report Number(s):: PNNL-SA--156131

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 3 Vol. 14; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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