Stabilizing Anionic Redox Chemistry in a Mn-Based Layered Oxide Cathode Constructed by Li-Deficient Pristine State

Cao, Xin; Li, Haifeng; Qiao, Yu; Jia, Min; Li, Xiang; Cabana, Jordi; Zhou, Haoshen

doi:10.1002/adma.202004280

Stabilizing Anionic Redox Chemistry in a Mn-Based Layered Oxide Cathode Constructed by Li-Deficient Pristine State

Journal Article · 01 January 2021 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202004280· OSTI ID:1804480

Cao, Xin; Li, Haifeng; Qiao, Yu; Jia, Min; Li, Xiang; Cabana, Jordi; Zhou, Haoshen

Li-rich cathode materials are of significant interest for coupling anionic redox with cationic redox chemistry to achieve high-energy-density batteries. However, lattice oxygen loss and derived structure distortion would induce serious capacity loss and voltage decay, further hindering its practical application. Herein, a novel Li-rich cathode material, O3-type Li_0.6[Li_0.2Mn_0.8]O₂, is developed with the pristine state displaying both a Li excess in the transition metal layer and a deficiency in the alkali metal layer. Benefiting from stable structure evolution and Li migration processes, not only can high reversible capacity (≈329 mAh g^-1) be harvested but also irreversible/reversible anionic/cationic redox reactions are comprehensively assigned via the combination of in/ex situ spectroscopies. Furthermore, irreversible lattice oxygen loss and structure distortion are effectively restrained, resulting in long-term cycle stability (capacity drop of 0.045% per cycle, 500 cycles). Altogether, tuning the Li state in the alkali metal layer presents a promising way for modification of high-capacity Li-rich cathode candidates.

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE) - Office of Vehicle Technologies (VTO); National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC); National Science Foundation (NSF)

DOE Contract Number:: AC02-06CH11357

OSTI ID:: 1804480

Journal Information:: Advanced Materials, Vol. 33, Issue 2

Publisher:: Wiley

Country of Publication:: United States

Language:: English

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