Direct Spectroscopy for Probing the Critical Role of Partial Covalency in Oxygen Reduction Reaction for Cobalt-Manganese Spinel Oxides
2019-04
Source PublicationNANOMATERIALS
ISSN2079-4991
Volume9Issue:4
Status已发表
DOI10.3390/nano9040577
AbstractNanocrystalline 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.
Keywordoxygen reduction reaction spinel oxides soft X-ray absorption spectroscopy partial covalency catalytic activity
Indexed BySCI ; SCIE
Language英语
Funding ProjectNational 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 Research AreaScience & Technology - Other Topics ; Materials Science
WOS SubjectNanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS IDWOS:000467768800093
PublisherMDPI
WOS KeywordX-RAY-ABSORPTION ; TRANSITION-METAL ; EVOLUTION REACTION ; ALKALINE-MEDIUM ; STATES ; ELECTROCATALYSIS ; FILMS ; HYBRIDIZATION ; ELECTRODES ; BATTERIES
Original Document TypeArticle
Citation statistics
Document Type期刊论文
Identifierhttps://kms.shanghaitech.edu.cn/handle/2MSLDSTB/40885
Collection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
Corresponding AuthorLiu, Xiaosong
Affiliation
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
Corresponding Author AffilicationSchool of Physical Science and Technology
Recommended Citation
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).
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