Lithiophilic Mo3N2/MoN as multifunctional interlayer for dendrite-free and ultra-stable lithium metal batteries

Xiaojuan Zhang; Yuanfu Chen; Katam Srinivas; Bo Yu; Fei Ma; Bin Wang; Xinqiang Wang; Jiarui He; Zheng-Long Xu

doi:10.1016/j.jcis.2021.12.143

Lithiophilic Mo₃N₂/MoN as multifunctional interlayer for dendrite-free and ultra-stable lithium metal batteries

J Colloid Interface Sci. 2022 Apr 15:612:332-341. doi: 10.1016/j.jcis.2021.12.143. Epub 2021 Dec 25.

Authors

Xiaojuan Zhang¹, Yuanfu Chen², Katam Srinivas³, Bo Yu³, Fei Ma³, Bin Wang³, Xinqiang Wang³, Jiarui He⁴, Zheng-Long Xu⁵

Affiliations

¹ School of Electronic Science and Engineering, and State Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 610054, PR China; Department of Industrial and Systems Engineering, The Hong Kong Polytechnic University, Hong Kong Special Administrative Region.
² School of Electronic Science and Engineering, and State Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 610054, PR China; School of Science, and Institute of Oxygen Supply, Tibet University, Lhasa, 850000, PR China. Electronic address: yfchen@uestc.edu.cn.
³ School of Electronic Science and Engineering, and State Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 610054, PR China.
⁴ School of Electronic Science and Engineering, and State Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 610054, PR China. Electronic address: hejiarui123@sina.com.
⁵ Department of Industrial and Systems Engineering, The Hong Kong Polytechnic University, Hong Kong Special Administrative Region. Electronic address: zhenglong.xu@polyu.edu.hk.

PMID: 34998193
DOI: 10.1016/j.jcis.2021.12.143

Abstract

The formation of lithium dendrite and the unstable electrode/electrolyte interface, especially at high rates, are the dominant obstacles impeding the implementation of lithium metal batteries (LMBs). To tackle these fundamental challenges, here we propose a lithiophilic Mo₃N₂/MoN heterostructure (designated as MoN_x) interlayer for dendrite-free and ultra-stable lithium metal anodes for the first time. The MoN_x interlayer presents excellent electrolyte wettability, fast lithium diffusion kinetics and strong mechanical strength, which function synergistically to inhibit lithium dendrite growth. During cycling, an in-situ formation of Li₃N-rich solid electrolyte interphase layer and metallic Mo phase can regulate the Li-ion conductivity and Li metal deposition, thus indicating uniform and compact Li plating. Above ameliorating features accompany an ultra-long-life of 2000 h at a high current density of 5 mA cm^-2 for the MoN_x-Li anode. The feasibility of the MoN_x-Li anode in LMB is further confirmed in conjunction with LiFePO₄ cathodes. The full cells deliver exceptionally high-capacity retentions of above 82.0% after 500 cycles at 1C and 425 cycles at 3C, which are among the best thus far reported for LMBs. This work provides both new insights towards functional interlayer design and effective transition-metal nitrides for practical LMBs.

Keywords: DFT calculations; In-situ reaction; Li(3)N-rich layer; Lithium metal batteries; Mo(3)N(2)/MoN heterostructure.