期刊
ADVANCED FUNCTIONAL MATERIALS
卷 32, 期 32, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202202853
关键词
catalyses; lithium-sulfur batteries; microassemblies; nanoalloys; shuttle effect
类别
资金
- National Natural Science Foundation of China [22109072]
- Natural Science Foundation of Jiangsu Province [BK20210349]
- China Postdoctoral Science Foundation [2021M691586]
- Postdoctoral Research Funding Scheme of Jiangsu Province [2021K446C]
- Natural Science Foundation of Hebei Province of China [B2021202028, B2020202052]
- Outstanding Youth Project of Guangdong Natural Science Foundation [2021B1515020051]
- Program for the Outstanding Young Talents of Hebei Province, China
- Department of Science and Technology of Guangdong Province [2020B0909030004, 2019JC01L203]
- Guangdong Innovative and Entrepreneurial Team Program [2016ZT06C517]
- Science and Technology Program of Guangzhou [2019050001]
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- University of Waterloo, and Waterloo Institute for Nanotechnology
In this work, a flower-like graphene microassembly decorated with finely-dispersed Ni2Co nanoalloy (Ni2Co@rGO) is developed as an advanced host matrix for Li-S batteries. The Ni2Co nanoalloys exhibit strong adsorbability against polysulfide shuttling and excellent catalytic activity for sulfur conversions. The sophisticated architecture of the microassembly facilitates electron/ion transport and highly-exposed active interfaces, enabling fast and durable sulfur electrochemistry. The use of Ni2Co@rGO as an anode matrix also improves the Li redox behavior.
Lithium-sulfur (Li-S) batteries present a promising solution to high-energy and low-cost energy storage. However, the conversion-type redox mechanism determines the poor fulfillment of battery chemistry in terms of reversibility and kinetics. Herein, a flower-like graphene microassembly decorated with finely-dispersed Ni2Co nanoalloy (Ni2Co@rGO) is developed as advanced host matrix for Li-S batteries. Combining computational, physicochemical, and electrochemical studies, Ni2Co nanoalloys are unveiled synergizing strong adsorbability against polysulfide shuttling and excellent catalytic activity for sulfur conversions. Meanwhile, the sophisticated architecture renders facile electron/ion transport and highly-exposed active interfaces. These virtues collaboratively contribute to fast and durable sulfur electrochemistry with a minimum capacity degradation of 0.034% per cycle over 500 cycles and a rate capability up to 5 C. Besides, the implementation of Ni2Co@rGO as the anode matrix tames the Li redox behavior benefiting from the enhanced lithiophilicity and reduced local current density. As such, the full cell configuration pairing S-Ni2Co@rGO cathode and Li-Ni2Co@rGO anode realizes a favorable areal capacity of 4.53 mAh cm(-2) under high sulfur loading (4.0 mg cm(-2)) and limited electrolyte (E/S = 6.0 mL g(-1)). This work offers an elaborate bi-service matrix engineering to simultaneously improve the conversion reversibility and kinetics for superior Li-S batteries.
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