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Surface-to-Bulk Redox Coupling through Thermally Driven Li Redistribution in Li- and Mn-Rich Layered Cathode Materials.
Li, Shaofeng; Lee, Sang-Jun; Wang, Xuelong; Yang, Wanli; Huang, Hai; Swetz, Daniel S; Doriese, William B; O'Neil, Galen C; Ullom, Joel N; Titus, Charles J; Irwin, Kent D; Lee, Han-Koo; Nordlund, Dennis; Pianetta, Piero; Yu, Chang; Qiu, Jieshan; Yu, Xiqian; Yang, Xiao-Qing; Hu, Enyuan; Lee, Jun-Sik; Liu, Yijin.
Afiliación
  • Li S; Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.
  • Lee SJ; State Key Lab of Fine Chemicals, School of Chemical Engineering, Liaoning Key Lab for Energy Materials and Chemical Engineering , Dalian University of Technology , Dalian 116024 , P. R. China.
  • Wang X; Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.
  • Yang W; Chemistry Division , Brookhaven National Laboratory , Upton , New York 11973 , United States.
  • Huang H; Beijing National Laboratory for Condensed Matter Physics, Institute of Physics , Chinese Academy of Sciences , Beijing 100190 , P. R. China.
  • Swetz DS; Advanced Light Source , Lawrence Berkeley National Laboratory , Berkeley , California 94720 , United States.
  • Doriese WB; Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.
  • O'Neil GC; National Institute of Standards and Technology , Boulder , Colorado 80305 , United States.
  • Ullom JN; National Institute of Standards and Technology , Boulder , Colorado 80305 , United States.
  • Titus CJ; National Institute of Standards and Technology , Boulder , Colorado 80305 , United States.
  • Irwin KD; National Institute of Standards and Technology , Boulder , Colorado 80305 , United States.
  • Lee HK; Department of Physics , Stanford University , Stanford , California 94305 , United States.
  • Nordlund D; Department of Physics , Stanford University , Stanford , California 94305 , United States.
  • Pianetta P; Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.
  • Yu C; Pohang Accelerator Laboratory , Pohang 37673 , Republic of Korea.
  • Qiu J; Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.
  • Yu X; Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.
  • Yang XQ; State Key Lab of Fine Chemicals, School of Chemical Engineering, Liaoning Key Lab for Energy Materials and Chemical Engineering , Dalian University of Technology , Dalian 116024 , P. R. China.
  • Hu E; State Key Lab of Fine Chemicals, School of Chemical Engineering, Liaoning Key Lab for Energy Materials and Chemical Engineering , Dalian University of Technology , Dalian 116024 , P. R. China.
  • Lee JS; Beijing National Laboratory for Condensed Matter Physics, Institute of Physics , Chinese Academy of Sciences , Beijing 100190 , P. R. China.
  • Liu Y; Chemistry Division , Brookhaven National Laboratory , Upton , New York 11973 , United States.
J Am Chem Soc ; 141(30): 12079-12086, 2019 Jul 31.
Article en En | MEDLINE | ID: mdl-31287957
Li- and Mn-rich (LMR) layered cathode materials have demonstrated impressive capacity and specific energy density thanks to their intertwined redox centers including transition metal cations and oxygen anions. Although tremendous efforts have been devoted to the investigation of the electrochemically driven redox evolution in LMR cathode at ambient temperature, their behavior under a mildly elevated temperature (up to ∼100 °C), with or without electrochemical driving force, remains largely unexplored. Here we show a systematic study of the thermally driven surface-to-bulk redox coupling effect in charged Li1.2Ni0.15Co0.1Mn0.55O2. We for the first time observed a charge transfer between the bulk oxygen anions and the surface transition metal cations under ∼100 °C, which is attributed to the thermally driven redistribution of Li ions. This finding highlights the nonequilibrium state and dynamic nature of the LMR material at deeply delithiated state upon a mild temperature perturbation.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2019 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2019 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos