Theoretical insights on alleviating lattice-oxygen evolution by sulfur substitution in Li_(1.2)Ni_(0.6)Mn_(0.2)O_(2) cathode material

作     者：Kuan-Yu Lin Santhanamoorthi Nachimuthu Han-Wen Huang Jyh-Chiang Jiang 

作者机构：Department of Chemical EngineeringNational Taiwan University of Science and TechnologyTaipeiTaiwanChina 

出 版 物：《npj Computational Materials》 (计算材料学（英文）)

年 卷 期：2022年第8卷第1期

页      面：2027-2036页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 08[工学] 0817[工学-化学工程与技术] 070303[理学-有机化学] 0703[理学-化学] 

基　　金：All the authors gratefully acknowledge the financial support from the Ministry of Science and Technology Taiwan(MOST 110-2639-E-011-001-ASP MOST 110-2923-E-011-002 and MOST 110-2923-M-011-003-MY2) 

主　　题：substitution sulfur insight 

摘      要：Here,we demonstrate that the lattice oxygen release on the high-capacity cathode,Li_(1.2)Ni_(0.6)Mn_(0.2)O_(2)(LNMO)surface can be successfully suppressed through S-anion-substitution using density functional theory(DFT)calculations and ab initio molecular dynamics(AIMD)*** oxygen evolution mechanisms on pristine and sulfur(S)-substituted LNMO(003)surfaces in the presence of an electrolyte mixture are ***-oxidation of O^(2−)anions during delithiation in the pristine surface results in oxygen evolution and subsequent structural ***,in the S-substituted LNMO,S^(2−)anions primarily participate in charge compensation and further inhibit oxygen evolution and O vacancy formation at high degrees of ***,the S-substitution effectively prevents the formation of Ni^(3+)ions and Jahn-Teller distortion,retaining the layered structure during *** findings provide insight into improving the structural stability of the LNMO(003)surface,paving the way for developing Li-rich LNMO cathode materials for next-generation LIBs.