Cho, Haneol Son, Hyunsu Kim, Donghun Lee, Minho Boateng, Samuel Han, HyukSu Kim, Kang Min Kim, Seungchul Choi, Heechae Song, Taeseup Lee, Kyu Hwan 2024-01-20T01:02:27Z 2024-01-20T01:02:27Z 2021-09-04 2017-07-20 1932-7447 https://pubs.kist.re.kr/handle/201004/122514 Li4Ti5O12 (LTO) has attracted tremendous attention as a stationary Li-ion battery anode material due to its excellent stability. However, the poor rate capability caused by the low electrical conductivity limits its practical use. Previously, Mg-doping in LTO has been used to improve the electrical conductivity and electrochemical properties, but the Mg-doped LTO system generally exhibits large anomalies in the electrical properties and capacities, which limits the reliable mass-production of engineered LTO. In this study, on the basis of first-principles calculations and related experiments, we systematically study the effects of charge-compensating point defects of the Mg-doped LTO on the electrical properties. A combination of first-principles calculations with thermodynamic modeling shows that high-temperature annealing under reducing conditions could effectively alter the Mg-doping site from a Ti4+ to Li+ site and increase the electrical conductivity significantly due to reduced electron effective mass and increased carrier concentration. Mg-doped LTO annealed under reducing condition exhibits a significantly improved rate compared capability with that of LTO annealed under air condition. The theoretical-analysis-associated experimental results provide more general design guidelines for the preparation of doped LTO with the promise of further improvements in performance. English American Chemical Society DOPED LI4TI5O12 ELECTROCHEMICAL PERFORMANCE COMPUTATIONAL PREDICTIONS LITHIUM BATTERIES DIFFUSION INSERTION DEFECTS STORAGE CARBON Impact of Mg-Doping Site Control in the Performance of Li4Ti5O12 Li-Ion Battery Anode: First-Principles Predictions and Experimental Verifications Article 10.1021/acs.jpcc.7b01475 1 The Journal of Physical Chemistry C, v.121, no.28, pp.14994 - 15001 The Journal of Physical Chemistry C 121 28 14994 15001 scie scopus 000406355700002 2-s2.0-85025461154 Chemistry, Physical Nanoscience & Nanotechnology Materials Science, Multidisciplinary Chemistry Science & Technology - Other Topics Materials Science Article DOPED LI4TI5O12 ELECTROCHEMICAL PERFORMANCE COMPUTATIONAL PREDICTIONS LITHIUM BATTERIES DIFFUSION INSERTION DEFECTS STORAGE CARBON