Issue 16, 2024

Optimizing interface concentration and electric fields for enhanced lithium deposition behavior in lithium metal anodes

Abstract

Understanding dynamic fluctuations in complex multi-physics fields at an electrolyte/electrode interface is crucial for explaining the lithium deposition mechanism and developing efficient interface structures, but there are significant challenges. Here, we introduce an internal standard substance (1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE)) to propose a quantitative in situ Raman spectroscopy method to disclose the variation of interfacial concentration field. It is proved that the formation of an anion depletion layer at the electrolyte/electrode interface during lithium deposition leads to the formation of a space charge layer (SCL) with local electric field, which can accelerate dendrite growth and is closely related to the withdrawal of anions from interface. Further, a high-anion-concentration interface (HACI) with immobilized anions is proposed. This HACI can effectively prevent anion depletion at the interface and enhance the interfacial Li+ transference number from 0.30 to 0.57, thus alleviating formation of SCL and facilitating uniform lithium deposition. Hence, a full cell with high-load NCM523 cathode (∼14 mg cm−2) and limited HACI@Li anode (∼50 μm) delivers excellent cycling over 200 cycles with a high discharge capacity retention of 77.6% (∼125.7 mA h g−1). This offers critical insights for designing lithium battery systems from the perspective of multi-physics fields.

Graphical abstract: Optimizing interface concentration and electric fields for enhanced lithium deposition behavior in lithium metal anodes

Supplementary files

Article information

Article type
Paper
Submitted
25 Apr 2024
Accepted
28 Jun 2024
First published
02 Jul 2024

Energy Environ. Sci., 2024,17, 5993-6002

Optimizing interface concentration and electric fields for enhanced lithium deposition behavior in lithium metal anodes

J. Liu, H. Hua, J. Lin, Y. Deng, N. Pei, P. Zhang, J. Dong, J. Li and J. Zhao, Energy Environ. Sci., 2024, 17, 5993 DOI: 10.1039/D4EE01816H

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