Quantification of Anionic Redox Chemistry in a Prototype Na-Rich Layered Oxide

Hu, Yue; Liu, Tiefeng; Cheng, Chen; Yan, Yingying; Ding, Manling; Chan, Ting-Shan; Guo, Jinghua; Zhang, Liang

doi:10.1021/acsami.9b19204

Quantification of Anionic Redox Chemistry in a Prototype Na-Rich Layered Oxide

Journal Article · Mon Dec 30 00:00:00 EST 2019 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.9b19204· OSTI ID:1780734

Hu, Yue ^[1]; Liu, Tiefeng ^[2]; Cheng, Chen ^[1]; Yan, Yingying ^[1]; Ding, Manling ^[1]; Chan, Ting-Shan ^[3]; ^[4]; ^[1]

Soochow Univ., Jiangsu (China)
Zhejiang Univ. of Technology (China)
National Synchrotron Radiation Research Center, Hsinchu (Taiwan)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Santa Cruz, CA (United States)

Harnessing anionic redox reactions is of prime importance for boosting the capacity of sodium-ion batteries (NIBs). However, quantifying the cyclability of anionic redox reactions is still challenging. Herein, we conduct a qualitative and quantitative investigation of the cationic and anionic redox reactions of a prototype Na-rich layered oxide, namely, Na₃RuO₄, by a combination of bulk-sensitive X-ray absorption spectroscopy and full-range mapping of resonant inelastic X-ray scattering. We unequivocally reveal that both Ru cations and oxygen anions are involved in the charge compensation process of Na₃RuO₄. Ru redox is highly reversible over extended electrochemical cycles, while the cyclability of lattice oxygen redox gradually decreases with the retention of only 36% after 30 cycles, which is mainly responsible for the capacity fading of Na₃RuO₄. Finally, our findings provide deeper insights into the complex oxygen redox mechanism, which plays a decisive role for designing high-energy Na-rich electrode materials for NIBs.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: Jiangsu Higher Education Institutions of China; National Natural Science Foundation of China (NNSFC); Natural Science Foundation of Jiangsu Province; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1780734

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 3 Vol. 12; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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resonant inelastic x-ray scattering
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