Self-consistent assessment of Li^(+) ion cathodes:Theory vs.experiments  

作　　者：Hongjie Xu Weidong Xiao Zhuo Wang Junhua Hu Guosheng Shao 

机构地区：[1]School of Materials Science and Engineering,Zhengzhou University,Zhengzhou 450001,China [2]Centre for International Cooperation on Designer Low-carbon&Environmental Materials(CDLCEM),Zhengzhou University,Zhengzhou 450001,China [3]Zhengzhou Materials Genome Institute(ZMGI),Zhengzhou 450100,China

出　　处：《Journal of Energy Chemistry》2021年第8期229-241,I0006,共14页能源化学（英文版）

基　　金：supported in part by the 1000 Talents Program of China;the Zhengzhou Materials Genome Institute;the National Natural Science Foundation of China(No.51001091,51571182,111174256,91233101,51602094,11274100);the Fundamental Research Program from the Ministry of Science and Technology of China(No.2014CB931704);the Program for Science&Technology Innovation Talents in the Universities of Henan Province(18HASTIT009)。

摘　　要：Transition metal oxide cathodes such as layered Li Co O_(2),spinel Li Mn_(2)O_(4) and olivine Li Fe PO4 have been commercialized for several decades and widely used in the rechargeable Li-ion batteries(LIBs).While great theoretical efforts have been made using the density functional theory(DFT)method,leading to insightful understanding covering materials stability and functional properties,the lack of consistency in choices of functionals and/or convergence criteria makes it somewhat difficult to compare results.It is therefore highly useful to assess these established systems towards self-consistency,thus offering a reliable working basis for theoretical formulation of novel cathodes.Here in this work,we have carried out systematic DFT calculations on the basis of recently established framework covering both thermodynamic stability,functional properties and associated mechanisms.Efforts have been made in selfconsistent selection of exchange-correlation(XC)functionals in terms of dependable accuracy with affordable computational cost,which is essential for high-throughput first-principles calculations.The outcome of the current work on three established cathode systems is in very good agreement with experimental data,and the methodology is to provide a solid basis for designing novel cathode materials without using costing non-local exchange-correlation functionals for structure-energy calculations.

关 键 词：Li-ion batteries Intercalation-type oxide cathodes Ab initio approaches SELF-CONSISTENCY Density functional theory 

分 类 号：TQ131.11[化学工程—无机化工] TM912[电气工程—电力电子与电力传动]