Direct Spectroscopy for Probing the Critical Role of Partial Covalency in Oxygen Reduction Reaction for Cobalt-Manganese Spinel Oxides

doi:10.3390/nano9040577

	Direct Spectroscopy for Probing the Critical Role of Partial Covalency in Oxygen Reduction Reaction for Cobalt-Manganese Spinel Oxides
	Long, Xinghui 1,2,3; Yu, Pengfei 1,2; Zhang, Nian 1,2; Li, Chun 4,5; Feng, Xuefei 6; Ren, Guoxi 1,2,3; Zheng, Shun 1,2,3; Fu, Jiamin1,2,7 ; Cheng, Fangyi 4,5; Liu, Xiaosong1,2,7
	2019-04
发表期刊	NANOMATERIALS (IF:4.4[JCR-2023],4.7[5-Year])
ISSN	2079-4991
卷号	9 期号:4
发表状态	已发表
DOI	10.3390/nano9040577
摘要	Nanocrystalline multivalent metal spinels are considered as attractive non-precious oxygen electrocatalysts. Identifying their active sites and understanding their reaction mechanisms are essential to explore novel transition metal (TM) oxides catalysts and further promote their catalytic efficiency. Here we report a systematic investigation, by means of soft X-ray absorption spectroscopy (sXAS), on cubic and tetragonal CoxMn3-xO4 (x = 1, 1.5, 2) spinel oxides as a family of highly active catalysts for the oxygen reduction reaction (ORR). We demonstrate that the ORR activity for oxide catalysts primarily correlates to the partial covalency of between O 2p orbital with Mn4+ 3d t(2g)-down/e(g)-up, Mn3+ 3d e(g)-up and Co3+ 3d e(g)-up orbitals in octahedron, which is directly revealed by the O K-edge sXAS. Our findings propose the critical influences of the partial covalency between oxygen 2p band and specific metal 3d band on the competition between intermediates displacement of the ORR, and thus highlight the importance of electronic structure in controlling oxide catalytic activity.
关键词	oxygen reduction reaction spinel oxides soft X-ray absorption spectroscopy partial covalency catalytic activity
收录类别	SCI ; SCIE
语种	英语
资助项目	National Natural Science Foundation of China[21473235] ; National Natural Science Foundation of China[U1632269] ; National Natural Science Foundation of China[11227902] ; National Natural Science Foundation of China[21503263]
WOS研究方向	Science & Technology - Other Topics ; Materials Science
WOS类目	Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:000467768800093
出版者	MDPI
WOS关键词	X-RAY-ABSORPTION ; TRANSITION-METAL ; EVOLUTION REACTION ; ALKALINE-MEDIUM ; STATES ; ELECTROCATALYSIS ; FILMS ; HYBRIDIZATION ; ELECTRODES ; BATTERIES
原始文献类型	Article
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/40885
专题	物质科学与技术学院_硕士生物质科学与技术学院_特聘教授组_刘啸嵩组
通讯作者	Liu, Xiaosong
作者单位	1.Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China 2.Chinese Acad Sci, CAS Ctr Excellence Superconducting Elect CENSE, Shanghai 200050, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Nankai Univ, Key Lab Adv Energy Mat Chem, Minist Educ, Tianjin 300071, Peoples R China 5.Nankai Univ, Coll Chem, State Key Lab Elementoorgan Chem, Tianjin 300071, Peoples R China 6.Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA 7.Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 200031, Peoples R China
通讯作者单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Long, Xinghui,Yu, Pengfei,Zhang, Nian,et al. Direct Spectroscopy for Probing the Critical Role of Partial Covalency in Oxygen Reduction Reaction for Cobalt-Manganese Spinel Oxides[J]. NANOMATERIALS,2019,9(4).
APA	Long, Xinghui.,Yu, Pengfei.,Zhang, Nian.,Li, Chun.,Feng, Xuefei.,...&Liu, Xiaosong.(2019).Direct Spectroscopy for Probing the Critical Role of Partial Covalency in Oxygen Reduction Reaction for Cobalt-Manganese Spinel Oxides.NANOMATERIALS,9(4).
MLA	Long, Xinghui,et al."Direct Spectroscopy for Probing the Critical Role of Partial Covalency in Oxygen Reduction Reaction for Cobalt-Manganese Spinel Oxides".NANOMATERIALS 9.4(2019).