Direct in situ measurements of electrical properties of solid-electrolyte interphase on lithium metal anodes

Yaobin Xu; Hao Jia; Peiyuan Gao; Diego E Galvez-Aranda; Saul Perez Beltran; Xia Cao; Phung M L Le; Jianfang Liu; Mark H Engelhard; Shuang Li; Gang Ren; Jorge M Seminario; Perla B Balbuena; Ji-Guang Zhang; Wu Xu; Chongmin Wang

doi:10.1038/s41560-023-01361-1

Direct in situ measurements of electrical properties of solid-electrolyte interphase on lithium metal anodes

Nat Energy. 2023 Dec;8(12):1345-1354. doi: 10.1038/s41560-023-01361-1. Epub 2023 Sep 28.

Authors

Yaobin Xu^{1

2}, Hao Jia^{3

2}, Peiyuan Gao⁴, Diego E Galvez-Aranda^{5

6}, Saul Perez Beltran⁵, Xia Cao³, Phung M L Le³, Jianfang Liu⁷, Mark H Engelhard¹, Shuang Li¹, Gang Ren⁷, Jorge M Seminario^{5

6

8}, Perla B Balbuena^{5

8

9}, Ji-Guang Zhang³, Wu Xu³, Chongmin Wang¹

Affiliations

¹ Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA, USA.
² These authors contributed equally: Yaobin Xu, Hao Jia.
³ Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, USA.
⁴ Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA, USA.
⁵ Department of Chemical Engineering, Texas A&M University, College Station, TX, USA.
⁶ Department of Electrical and Computer Engineering, Texas A&M University, College Station, TX, USA.
⁷ The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
⁸ Department of Materials Science and Engineering, Texas A&M University, College Station, TX, USA.
⁹ Department of Chemistry, Texas A&M University, College Station, TX, USA.

Abstract

The solid-electrolyte interphase (SEI) critically governs the performance of rechargeable batteries. An ideal SEI is expected to be electrically insulative to prevent persistently parasitic reactions between the electrode and the electrolyte and ionically conductive to facilitate Faradaic reactions of the electrode. However, the true nature of the electrical properties of the SEI remains hitherto unclear due to the lack of a direct characterization method. Here we use in situ bias transmission electron microscopy to directly measure the electrical properties of SEIs formed on copper and lithium substrates. We reveal that SEIs show a voltage-dependent differential conductance. A higher rate of differential conductance induces a thicker SEI with an intricate topographic feature, leading to an inferior Coulombic efficiency and cycling stability in Li∣∣Cu and Li∣∣LiNi_0.8Mn_0.1Co_0.1O₂ cells. Our work provides insight into the targeted design of the SEI with desired characteristics towards better battery performance.

Abstract

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