Engineering catalytic defects via molecular imprinting for high energy Li-S pouch cells

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外文摘要：Heterogeneous catalysis promises to accelerate sulfur-involved conversion reactions in lithium-sulfur batteries.Solid-state Li2S dissociation remains as the rate-limiting step because of the weakly matched solid-solid electrocatalysis interfaces.We propose an electrochemically molecular-imprinting strategy to have a metal sulfide(MS)catalyst with imprinted defects in positions from which the pre-implanted Li2S has been electrochemically removed.Such tailor-made defects enable the catalyst to bind exclusively to Li atoms in Li2S reactant and elongate the Li-S bond,thus decreasing the reaction energy barrier during charging.The imprinted Ni3S2 catalyst shows the best activity due to the highest defect concentration among the MS catalysts examined.The Li2S oxidation potential is substantially reduced to 2.34 V from 2.96 V for the counterpart free of imprinted vacancies,and an Ah-level pouch cell is realized with excellent cycling performance.With a lean electrolyte/sulfur ratio of 1.80 μL mgs-1,the cell achieves a benchmarkedly high energy density beyond 500 Wh kg-1.

外文关键词：

lithium-sulfur batterycatalystsdefectsenergy densitymetal sulfide

作者：

Yufei Zhao、Chuannan Geng、Li Wang、Yun Cao、Haotian Yang、Linkai Peng、Xin Jiang、Yong Guo、Xiaolin Ye、Wei Lv、Quan-Hong Yang

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作者单位：

Shenzhen Geim Graphene Center,Engineering Laboratory for Functionalized Carbon Materials,Tsinghua Shenzhen International Graduate School,Tsinghua University,Shenzhen 518055,China

Nanoyang Group,Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage,School of Chemical Engineering and Technology,and Collaborative Innovation Center of Chemical Science and Engineering(Tianjin),Tianjin University,Tianjin 300072,China

Joint School of National University of Singapore and Tianjin University,In

Joint School of National University of Singapore and Tianjin University,International Campus of Tianjin University,Fuzhou 350207,China

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基金：

National Key Research and Development Program of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaShenzhen Science and Technology ProgramHaihe Laboratory of Sustainable Chemical Transformations,the Fundamental Research Funds for the Central UniversitiesChina Postdoctoral Science Foundation

项目编号：

2021YFF0500600519320055202204152302300JCYJ202208181010080182022M722361

出版年：

2024

DOI：

10.1093/nsr/nwae190

国家科学评论(英文版)

CSTPCD

ISSN：

年,卷(期)：2024.11(7)

参考文献量2