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Surface-to-Bulk Redox Coupling Through Thermally Driven Li Redistribution in Li- And Mn-Rich Layered Cathode Materials

Surface-to-Bulk Redox Coupling Through Thermally Driven Li Redistribution in Li- And Mn-Rich Layered Cathode Materials

Shaofeng Li, Sang-Jun Lee, Xuelong Wang, Wanli Yang, Hai Huang, Daniel S Swetz, William B Doriese, Galen C O'Neil, Joel N Ullom, Charles J Titus, Kent D Irwin, Han-Koo Lee, Dennis Nordlund, Piero Pianetta, etc.

J Am Chem Soc. 2019 Jul 31;141(30):12079-12086.

PMID: 31287957

Abstract:

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.

Chemicals Related in the Paper:

Catalog Number	Product Name	Structure	CAS Number	Price
AS212704	Density Standard (100 °C)			Price

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