Unprecedented strong and reversible atomic orbital hybridization enables a highly stable Li–S battery  

作　　者：Min Yan Wenda Dong Fu Liu Lihua Chen Tawfique Hasan Yu Li Bao-Lian Su 

机构地区：[1]State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China [2]Hubei Key Laboratory of Plasma Chemistry and Advanced Materials,Hubei Engineering Technology Research Center of Optoelectronic and New Energy Materials,School of Materials Science and Engineering,Wuhan Institute of Technology,Wuhan 430205,China [3]School of Materials Science and Engineering,Zhejiang University,Hangzhou 310027,China [4]Cambridge Graphene Centre,University of Cambridge,Cambridge CB30FA,UK [5]Laboratory of Inorganic Materials Chemistry(CMI),University of Namur,Namur B-5000,Belgium

出　　处：《National Science Review》2022年第7期109-119,共11页国家科学评论（英文版）

基　　金：supported by the National Key R&D Program of China (2016YFA0202602 and 2021YFE0115800);the National Natural Science Foundation of China (U1663225, U20A20122and 52103285);the Program for Changjiang Scholars and Innovative Research Team in University (IRT 15R52) of the Ministry of Education of China;the Program of Introducing Talents of Discipline to Universities-Plan 111 (B20002) from the Ministry of Science and Technology and the Ministry of Education of China;the Natural Science Foundation of Hubei Province(2021CFB082 and 2020CFB416);the Scientific Research Foundation of Wuhan Institute of Technology (K2021042);the Open Key Fund Project of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology, 2022-KF-10).

摘　　要：The shuttle effect and excessive volume change of the sulfur cathode severely impede the industrial implementation of Li–S batteries.It is still highly challenging to find an efficient way to suppress the shuttle effect and volume expansion.Here,we report,for the first time,an innovative atomic orbital hybridization concept to construct the hierarchical hollow sandwiched sulfur nanospheres with double-polyaniline layers as the cathode material for large-scale high-performance Li–S batteries.This hierarchically 3D,cross-linked and stable sulfur–polyaniline backbone with interconnected disulfide bonds provides a new type and strong intrinsic chemical confinement of sulfur owing to the atomic orbital hybridization of Li 2s,S 3p,C 2p and N 2p.Crucially,such atomic orbital hybridization of sulfur sandwiched in the double sulfur–polyaniline network is highly reversible during the discharge/charge process and can very efficiently suppress the shuttle effect and volume expansion,contributing to a very high capacity of 1142 mAh g^(–1)and an excellent stabilized capacity of 886 mAh g^(–1)at 0.2 C after 500 cycles with a suppressed volume expansion and an unprecedented electrode integrity.This innovative atomic orbital hybridization concept can be extended to the preparation of other electrode materials to eliminate the shuttle effect and volume expansion in battery technologies.The present work also provides a commercially viable and up-scalable cathode material based on this strong and highly reversible atomic orbital hybridation for large-scale high-performance Li–S batteries.

关 键 词：atomic orbital hybridization hierarachical hollow sandwiched sulfur nanosphere double sulfur-polyaniline networks lithium-sulfur batteries in situ vulcanization 

分 类 号：TM912[电气工程—电力电子与电力传动] O646[理学—物理化学]