Exploring Oxygen Activity in the High Energy P2-Type Na0.78Ni0.23Mn0.69O2 Cathode Material for Na-Ion Batteries

Ma, Chuze; Alvarado, Judith; Xu, Jing; Clément, Raphaële J.; Kodur, Moses; Tong, Wei; Grey, Clare P.; Meng, Ying Shirley

doi:10.1021/jacs.7b00164

Title: Exploring Oxygen Activity in the High Energy P2-Type Na_0.78Ni_0.23Mn_0.69O₂ Cathode Material for Na-Ion Batteries

Journal Article · 21 March 2017 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.7b00164 · OSTI ID:1532243

Ma, Chuze ^[1]; Alvarado, Judith ^[1]; Xu, Jing ^[2]; Clément, Raphaële J. ^[3]; Kodur, Moses ^[1];

^[4]; Grey, Clare P. ^[3];

^[1]

Univ. of California, San Diego, CA (United States). Dept. of NanoEngineering
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Iowa State Univ., Ames, IA (United States)
Univ. of Cambridge (United Kingdom)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Large-scale electric energy storage is fundamental to the use of renewable energy. Recently, research and development efforts on room-temperature sodium-ion batteries (NIBs) have been revitalized, as NIBs are considered promising, low-cost alternatives to the current Li-ion battery technology for large-scale applications. Herein, we introduce a novel layered oxide cathode material, Na_0.78Ni_0.23Mn_0.69O₂. This new compound provides a high reversible capacity of 138 mAh g^-1 and an average potential of 3.25 V vs Na⁺/Na with a single smooth voltage profile. Its remarkable rate and cycling performances are attributed to the elimination of the P2-O2 phase transition upon cycling to 4.5 V. The first charge process yields an abnormally excess capacity, which has yet to be observed in other P2 layered oxides. Metal K-edge XANES results show that the major charge compensation at the metal site during Na-ion deintercalation is achieved via the oxidation of nickel (Ni²⁺) ions, whereas, to a large extent, manganese (Mn) ions remain in their Mn⁴⁺ state. Interestingly, electron energy loss spectroscopy (EELS) and soft X-ray absorption spectroscopy (sXAS) results reveal differences in electronic structures in the bulk and at the surface of electrochemically cycled particles. At the surface, transition metal ions (TM ions) are in a lower valence state than in the bulk, and the O K-edge prepeak disappears. On the basis of previous reports on related Li-excess LIB cathodes, it is proposed that part of the charge compensation mechanism during the first cycle takes place at the lattice oxygen site, resulting in a surface to bulk transition metal gradient. We believe that by optimizing and controlling oxygen activity, Na layered oxide materials with higher capacities can be designed.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515

OSTI ID:: 1532243

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 13 Vol. 139; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Exploring Oxygen Activity in the High Energy P2-Type Na_0.78Ni_0.23Mn_0.69O₂ Cathode Material for Na-Ion Batteries