High Interfacial-Energy Interphase Promoting Safe Lithium Metal Batteries

Liu, Sufu; Ji, Xiao; Yue, Jie; Hou, Singyuk; Wang, Pengfei; Cui, Chunyu; Chen, Ji; Shao, Bowen; Li, Jingru; Han, Fudong; Tu, Jiangping; Wang, Chunsheng

doi:10.1021/jacs.9b11750

High Interfacial-Energy Interphase Promoting Safe Lithium Metal Batteries

Journal Article · Sun Jan 12 04:00:00 EST 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b11750· OSTI ID:1799451

Liu, Sufu ^[1]; Ji, Xiao ^[2]; Yue, Jie ^[2]; Hou, Singyuk ^[2]; ^[2]; Cui, Chunyu ^[2]; ^[2]; Shao, Bowen ^[3]; Li, Jingru ^[4]; ^[3]; ^[4]; ^[2]

University of Maryland, College Park, MD (United States); Zhejiang University, Hangzhou (China); University of Maryland
University of Maryland, College Park, MD (United States)
Rensselaer Polytechnic Institute, Troy, NY (United States)
Zhejiang University, Hangzhou (China)

We report engineering a stable solid electrolyte interphase (SEI) is critical for suppression of lithium dendrites. However, formation of desired SEI by formulating electrolyte composition is very difficult due to complex electrochemical reduction reactions. Here, instead of try-and-error of electrolyte composition, we design a Li-11 wt% Sr alloy anode to form SrF₂-rich SEI in fluorinated electrolytes. Density functional theory (DFT) calculation and experimental characterization demonstrate that SrF₂-rich SEI has a large interfacial energy with Li metal and a high mechanical strength, which can effectively suppress the Li dendrite growth by simultaneously promoting the lateral growth of deposited Li metal and the SEI stability. The Li-Sr/Cu cells in 2M LiFSI-DME shows an outstanding Li plating/stripping Coulombic efficiency of 99.42% at 1 mA cm^-2 with a capacity of 1 mAh cm^-2 and 98.95% at 3 mA cm^-2 with a capacity of 2 mAh cm^-2, respectively. The symmetric Li-Sr/Li-Sr cells also achieve a stable electrochemical performance of 180 cycles at an extremely high current density of 30 mA cm^-2 with a capacity of 1 mAh cm^-2. When paired with LiFePO₄ (LFP) and LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathodes, Li-Sr/LFP cells in 2M LiFSI-DME electrolytes and Li-Sr/NMC811 cells in 1M LiPF₆ in FEC:FEMC:HFE electrolytes also maintain excellent capacity retention. Designing SEI by regulating Li metal anode composition opens up a new and rational avenue to suppress Li dendrites.

View Accepted Manuscript (DOE)

Research Organization:: University of Maryland, College Park, MD (United States); Rensselaer Polytechnic Institute, Troy, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0008202

OSTI ID:: 1799451

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 5 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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High Interfacial-Energy Interphase Promoting Safe Lithium Metal Batteries

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