Deciphering the defect micro‐environment of graphene for highly efficient Li–S redox reactions
Yingze Song,
Hua Gao,
Menglei Wang,
Le Chen,
Xuan Cao,
Lixian Song,
Xiaohong Liu,
Wenlong Cai,
Jingyu Sun,
Wei Zhang
Affiliations
Yingze Song
State Key Laboratory of Environment‐Friendly Energy Materials, School of Materials and Science Engineering Southwest University of Science and Technology Mianyang Sichuan China
Hua Gao
State Key Laboratory of Environment‐Friendly Energy Materials, School of Materials and Science Engineering Southwest University of Science and Technology Mianyang Sichuan China
Menglei Wang
College of Energy, Soochow Institute for Energy and Materials Innovations, Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province Soochow University Suzhou Jiangsu China
Le Chen
State Key Laboratory of Environment‐Friendly Energy Materials, School of Materials and Science Engineering Southwest University of Science and Technology Mianyang Sichuan China
Xuan Cao
State Key Laboratory of Environment‐Friendly Energy Materials, School of Materials and Science Engineering Southwest University of Science and Technology Mianyang Sichuan China
Lixian Song
State Key Laboratory of Environment‐Friendly Energy Materials, School of Materials and Science Engineering Southwest University of Science and Technology Mianyang Sichuan China
Xiaohong Liu
Chongqing Institute of Green and Intelligent Technology Chinese Academy of Sciences Chongqing China
Wenlong Cai
Department of Advanced Energy Materials, College of Materials Science and Engineering Sichuan University Chengdu Sichuan China
Jingyu Sun
College of Energy, Soochow Institute for Energy and Materials Innovations, Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province Soochow University Suzhou Jiangsu China
Wei Zhang
Chongqing Institute of Green and Intelligent Technology Chinese Academy of Sciences Chongqing China
Abstract The lithium polysulfides (LiPS) dissolution into electrolyte as well as consequent shuttle behavior seriously exacerbate the electrochemical performance of lithium–sulfur batteries. Herein, the intrinsic defect of graphene has been tailored by using plasma irradiation. The topological defective carbon structure is demystified into monovacancy and divacancy which effectively promote Li–S redox kinetics by selectively decelerating the generation of soluble high‐order LiPSs and passingly promoting the conversion to final solid products. Theoretical prediction uncovers the selective manipulation of Li–S redox kinetics by defective graphene, facilitating the reduced overpotential effect and uniform deposition of Li2S. Moreover, the divacancy presents a higher activity for Li–S chemistry in contrast with monovacancy. Therefore, the battery achieves superior cyclability with a capacity retention of 88.6% at 1.0 C over 300 cycles. Furthermore, it yields an areal capacity up to 8.5 mAh cm−2 with a sulfur loading of 13.3 mg cm−2.
