Suppressing electrolyte-lithium metal reactivity via Li+-desolvation in uniform nano-porous separator

Sheng, Li; Wang, Qianqian; Liu, Xiang; Cui, Hao; Wang, Xiaolin; Xu, Yulong; Li, Zonglong; Wang, Li; Chen, Zonghai; Xu, Gui-Liang; Wang, Jianlong; Tang, Yaping; Amine, Khalil; Xu, Hong; He, Xiangming

doi:10.1038/s41467-021-27841-0

Suppressing electrolyte-lithium metal reactivity via Li⁺-desolvation in uniform nano-porous separator

Journal Article · Mon Jan 10 00:00:00 UTC 2022 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-27841-0· OSTI ID:1841749

Sheng, Li ^[1]; Wang, Qianqian ^[1]; Liu, Xiang ^[2]; Cui, Hao ^[1]; Wang, Xiaolin ^[1]; Xu, Yulong ^[1]; Li, Zonglong ^[1]; Wang, Li ^[1]; Chen, Zonghai ^[2]; Xu, Gui-Liang ^[2]; Wang, Jianlong ^[1]; Tang, Yaping ^[1]; Amine, Khalil ^[3]; Xu, Hong ^[1]; He, Xiangming ^[1]

Tsinghua Univ., Beijing (China)
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Stanford Univ., CA (United States)

Lithium reactivity with electrolytes leads to their continuous consumption and dendrite growth, which constitute major obstacles to harnessing the tremendous energy of lithium-metal anode in a reversible manner. Considerable attention has been focused on inhibiting dendrite via interface and electrolyte engineering, while admitting electrolyte-lithium metal reactivity as a thermodynamic inevitability. Here, we report the effective suppression of such reactivity through a nano-porous separator. Calculation assisted by diversified characterizations reveals that the separator partially desolvates Li⁺ in confinement created by its uniform nanopores, and deactivates solvents for electrochemical reduction before Li⁰-deposition occurs. The consequence of such deactivation is realizing dendrite-free lithium-metal electrode, which even retaining its metallic lustre after long-term cycling in both Li-symmetric cell and high-voltage Li-metal battery with LiNi_0.6Mn_0.2Co_0.2O₂ as cathode. The discovery that a nano-structured separator alters both bulk and interfacial behaviors of electrolytes points us toward a new direction to harness lithium-metal as the most promising anode.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Ministry of Science and Technology of the Republic of China (MOST); National Natural Science Foundation of China (NSFC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1841749

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 13; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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