Please use this identifier to cite or link to this item: https://hdl.handle.net/2440/124245
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Type: Journal article
Title: Revealing principles for design of lean-electrolyte lithium metal anode via In situ spectroscopy
Author: Li, H.
Chao, D.
Chen, B.
Chen, X.
Chuah, C.
Tang, Y.
Jiao, Y.
Jaroniec, M.
Qiao, S.-Z.
Citation: Journal of the American Chemical Society, 2020; 142(4):2012-2022
Publisher: American Chemical Society
Issue Date: 2020
ISSN: 0002-7863
1520-5126
Statement of
Responsibility: 
Huan Li, Dongliang Chao, Biao Chen, Xiao Chen, Clarence Chuah, Youhong Tang, Yan Jiao, Mietek Jaroniec and Shi-Zhang Qiao
Abstract: Lean-electrolyte conditions are highly pursued for practical lithium (Li) metal batteries. The previous studies on the Li metal anodes, in general, exhibited good stability with a large excess of electrolyte. However, the targeted design of Li hosts under relatively low electrolyte conditions has been rarely studied so far. Herein, we have shown that electrolyte consumption severely affects the cycling stability of Li metal anode. Considering carbon hosts as typical examples, we innovatively employed in situ synchrotron X-ray diffraction, in situ Raman spectroscopy, and theoretical computations to obtain a better understanding of the Li nucleation/deposition processes. We also showed the usefulness of in situ electrochemical impedance spectra to analyze interfacial fluctuation at the Li/electrolyte interface, together with nuclear magnetic resonance data to quantify electrolyte consumption. We have found that uneven Li nucleation/deposition and the crack of surface-area-derived solid-electrolyte interface (SEI) layer both lead to a great consumption of electrolyte. Then, we suggested a design principle for Li host to overcome the electrolyte loss, that is, uneven growth of the Li structure and the crack of the SEI layer must be simultaneously controlled. As a proof of concept, we demonstrated the usefulness of a 3D low-surface-area defective graphene host (L-DG) to control Li nucleation/deposition and stabilize the SEI layer, contributing to a highly reversible Li plating/stripping. As a result, such a Li host can achieve stable cycles (e.g., 1.0 mAh cm-2) with a low electrolyte loading (10 μL). This work demonstrates the necessity to design Li metal anodes under lean-electrolyte conditions and brings Li metal batteries a step closer to their practical applications.
Keywords: Electrodes; surface chemistry; defects; electrolytes; nucleation
Rights: © 2020 American Chemical Society
DOI: 10.1021/jacs.9b11774
Grant ID: http://purl.org/au-research/grants/arc/DP160104866
http://purl.org/au-research/grants/arc/LP160100927
http://purl.org/au-research/grants/arc/FL170100154
Appears in Collections:Aurora harvest 4
Chemical Engineering publications

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