气候变化领域集成服务门户(CCPortal): Multiorbital bond formation for stable oxygen-redox reaction in battery electrodes

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DOI	10.1039/c9ee04197d
	Multiorbital bond formation for stable oxygen-redox reaction in battery electrodes
	Sudayama T.; Uehara K.; Mukai T.; Asakura D.; Shi X.-M.; Tsuchimoto A.; Mortemard De Boisse B.; Shimada T.; Watanabe E.; Harada Y.; Nakayama M.; Okubo M.; Yamada A.
发表日期	2020
ISSN	1754-5692
起始页码	1492
结束页码	1500
卷号	13 期号:5
英文摘要	High-energy-density batteries have been a long-standing target toward sustainability, but the energy density of state-of-the-art lithium-ion batteries is limited in part by the small capacity of the positive electrode materials. Although employing the additional oxygen-redox reaction of Li-excess transition-metal oxides is an attractive approach to increase the capacity, an atomic-level understanding of the reaction mechanism has not been established so far. Here, using bulk-sensitive resonant inelastic X-ray scattering spectroscopy combined with ab initio computations, we demonstrate the presence of a localized oxygen 2p orbital weakly hybridized with transition metal t2g orbitals that was theoretically predicted to play a key role in oxygen-redox reactions. After oxygen oxidation, the hole in the oxygen 2p orbital is stabilized by the generation of either a (σ + π) multiorbital bond through strong π back-donation or peroxide O22- through oxygen dimerization. The multiorbital bond formation with σ-accepting and π-donating transition metals can thus lead to reversible oxygen-redox reaction. © The Royal Society 2020 of Chemistry.
语种	英语
scopus关键词	Chemical bonds; Electrodes; Lithium compounds; Lithium-ion batteries; Oxygen; Transition metal oxides; Transition metals; X ray scattering; Ab initio computations; Battery electrode; Bulk sensitive; High-energy density batteries; Oxygen redox reactions; Positive electrode materials; Reaction mechanism; Resonant inelastic x-ray scattering; Redox reactions; chemical bonding; chemical reaction; electrode; equipment; oxygen; redox conditions
来源期刊	Energy and Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/162783
作者单位	Research Institute for Energy Conservation, National Institute of Advanced Industrial Science and Technology, Tsukuba, Ibaraki, 305-8568, Japan; Department of Chemical System Engineering, School of Engineering, University of Tokyo, Bunkyo-ku, Tokyo, 113-8656, Japan; Frontier Research Institute for Materials Science (FRIMS), Nagoya Institute of Technology, Showa-ku, Nagoya, Aichi, 466-8555, Japan; Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, Nishikyo-ku, Kyoto, 615-8245, Japan; Institute for Solid State Physics, University of Tokyo, Kashiwa, Chiba, 277-8581, Japan; Mi2i Green, National Institute of Materials Science (NIMS), Tsukuba, Ibaraki, 305-0047, Japan
推荐引用方式 GB/T 7714	Sudayama T.,Uehara K.,Mukai T.,et al. Multiorbital bond formation for stable oxygen-redox reaction in battery electrodes[J],2020,13(5).
APA	Sudayama T..,Uehara K..,Mukai T..,Asakura D..,Shi X.-M..,...&Yamada A..(2020).Multiorbital bond formation for stable oxygen-redox reaction in battery electrodes.Energy and Environmental Science,13(5).
MLA	Sudayama T.,et al."Multiorbital bond formation for stable oxygen-redox reaction in battery electrodes".Energy and Environmental Science 13.5(2020).