Ahn, Jinho Kang, Jungmin Cho, Min-kyung Park, Hyunyoung Ko, Wonseok Lee, Yongseok Kim, Hyun-Soo Jung, Young Hwa Jeon, Tae-Yeol Kim, Hyungsub Ryu, Won-Hee Hong, Jihyun Kim, Jongsoon 2024-01-19T13:04:19Z 2024-01-19T13:04:19Z 2022-01-10 2021-12 1614-6832 https://pubs.kist.re.kr/handle/201004/116007 Despite their high energy densities, Li-rich layered oxides suffer from low capacity retention and continuous voltage decay caused by the migration of transition-metal cations into the Li layers. The cation migration stabilizes oxidized oxygen anions through the decoordination of oxygen from the metal once the anions participate in the redox reaction. Structural disordering is thus considered inevitable in most Li-rich layered oxides. However, herein, a Mg-substituted Li-rich layered oxide, Li1.2Mg0.2Ru0.6O2, with high structural and electrochemical stability is presented. Although using both cationic and anionic redox reactions, Ru migration in Li1.2-xMg0.2Ru0.6O2 is thermodynamically unfavored as a result of selectively oxidized O ions, suppressed structural disordering, and the formation of short (1.75 angstrom) Ru=O bonds enabled within the layered framework, which effectively decoordinate the oxidized O ions. The unprecedentedly high structural stability of Li1.2Mg0.2Ru0.6O2 leads to not only a high energy density of 964 Wh kg(-1) but also outstanding rate capability and cycle performance. These findings demonstrate the potential of this practical strategy for the stabilization of Li-rich layered oxides even with prolonged cycling. English WILEY-V C H VERLAG GMBH HIGH-CAPACITY LITHIUM DIFFUSION DENSITY ELECTROLYTES ORIGIN SOFT Selective Anionic Redox and Suppressed Structural Disordering Enabling High-Energy and Long-Life Li-Rich Layered-Oxide Cathode Article 10.1002/aenm.202102311 1 ADVANCED ENERGY MATERIALS, v.11, no.47 ADVANCED ENERGY MATERIALS 11 47 scie scopus 000711818900001 2-s2.0-85117930741 Chemistry, Physical Energy & Fuels Materials Science, Multidisciplinary Physics, Applied Physics, Condensed Matter Chemistry Energy & Fuels Materials Science Physics Article HIGH-CAPACITY LITHIUM DIFFUSION DENSITY ELECTROLYTES ORIGIN SOFT anionic redox cation migration first-principles calculations high energy density Li-ion batteries Li-rich layered oxides