TY - JOUR
T1 - Revealing Principles for Design of Lean-Electrolyte Lithium Metal Anode via in Situ Spectroscopy
AU - Li, Huan
AU - Chao, Dongliang
AU - Chen, Biao
AU - Chen, Xiao
AU - Chuah, Clarence
AU - Tang, Youhong
AU - Jiao, Yan
AU - Jaroniec, Mietek
AU - Qiao, Shi Zhang
PY - 2020/1/3
Y1 - 2020/1/3
N2 - 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.
AB - 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.
KW - Principles for Design
KW - Lean-Electrolyte
KW - Metal Anode
KW - Situ Spectroscopy
UR - http://www.scopus.com/inward/record.url?scp=85078346418&partnerID=8YFLogxK
UR - http://purl.org/au-research/grants/arc/DP160104866
UR - http://purl.org/au-research/grants/arc/LP160100927
UR - http://purl.org/au-research/grants/arc/FL170100154
U2 - 10.1021/jacs.9b11774
DO - 10.1021/jacs.9b11774
M3 - Article
C2 - 31898901
AN - SCOPUS:85078346418
VL - 142
SP - 2012
EP - 2022
JO - Journal of The American Chemical Society
JF - Journal of The American Chemical Society
SN - 0002-7863
IS - 4
ER -