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Discriminating Catalytically Active FeNx Species of Atomically Dispersed Fe-N-C Catalyst for Selective Oxidation of the C-H Bond
Liu, Wengang1,2; Zhang, Leilei1; Liu, Xin1; Liu, Xiaoyan1; Yang, Xiaofeng1; Miao, Shu1; Wang, Wentao1; Wang, Aiqin1; Zhang, Tao1
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2017-08-09
DOI10.1021/jacs.7b05130
Volume139Issue:31Pages:10790-10798
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Multidisciplinary
WOS Research AreaChemistry
WOS KeywordOXYGEN REDUCTION REACTION ; SINGLE-ATOM CATALYST ; NITROGEN-DOPED GRAPHENE ; FUEL-CELLS ; CHEMOSELECTIVE HYDROGENATION ; HETEROGENEOUS CATALYSIS ; METAL-CATALYSTS ; POROUS CARBON ; IRON ; NANOPARTICLES
AbstractNanostructured Fe-N-C materials represent a new type of "platinum-like" non-noble-metal catalyst for various electrochemical reactions and organic transformations. However, no consensus has been reached on the active sites of the Fe-N-C catalysts because of their heterogeneity in particle size and composition. In this contribution, we have successfully prepared atomically dispersed Fe-N-C catalyst, which exhibited high activity and excellent reusability for the selective oxidation of the C-H bond. A wide scope of substrates, including aromatic, heterocyclic, and aliphatic alkanes, were smoothly oxidized at room temperature, and the selectivity of corresponding products reached as high as 99%. By using sub-angstrom-resolution HAADF-STEM in combination with XPS, XAS, ESR, and Mossbauer spectroscopy, we have provided solid evidence that Fe is exclusively, dispersed as single atoms via forming FeNx (x = 4-6) and that the, relative concentration of each FeNx species is critically dependent on the pyrolysis temperature. Among them, the medium-spin (FeN5)-N-III affords the highest turnover frequency (6455 h(-1)), which is at least 1 order of magnitude more active than the high-spin and low-spin (FeN6)-N-III structures and 3 times More active than the (FeN4)-N-II structure, although its relative concentration in the catalysts is much lower than that of the (FeN6)-N-III structures.
Language英语
WOS IDWOS:000407540200034
Citation statistics
Cited Times:86[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/149806
Collection中国科学院大连化学物理研究所
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, iChEM Collaborat Innovat Ctr Chem Energy Mat, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
Recommended Citation
GB/T 7714
Liu, Wengang,Zhang, Leilei,Liu, Xin,et al. Discriminating Catalytically Active FeNx Species of Atomically Dispersed Fe-N-C Catalyst for Selective Oxidation of the C-H Bond[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2017,139(31):10790-10798.
APA Liu, Wengang.,Zhang, Leilei.,Liu, Xin.,Liu, Xiaoyan.,Yang, Xiaofeng.,...&Zhang, Tao.(2017).Discriminating Catalytically Active FeNx Species of Atomically Dispersed Fe-N-C Catalyst for Selective Oxidation of the C-H Bond.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,139(31),10790-10798.
MLA Liu, Wengang,et al."Discriminating Catalytically Active FeNx Species of Atomically Dispersed Fe-N-C Catalyst for Selective Oxidation of the C-H Bond".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 139.31(2017):10790-10798.
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