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题名: Discriminating Catalytically Active FeNx Species of Atomically Dispersed Fe-N-C Catalyst for Selective Oxidation of the C-H Bond
作者: Liu, Wengang1, 2;  Zhang, Leilei1;  Liu, Xin1;  Liu, Xiaoyan1;  Yang, Xiaofeng1;  Miao, Shu1;  Wang, Wentao1;  Wang, Aiqin1;  Zhang, Tao1
刊名: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
发表日期: 2017-08-09
DOI: 10.1021/jacs.7b05130
卷: 139, 期:31, 页:10790-10798
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Multidisciplinary
研究领域[WOS]: Chemistry
英文摘要: Nanostructured 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.
关键词[WOS]: OXYGEN REDUCTION REACTION ;  SINGLE-ATOM CATALYST ;  NITROGEN-DOPED GRAPHENE ;  FUEL-CELLS ;  CHEMOSELECTIVE HYDROGENATION ;  HETEROGENEOUS CATALYSIS ;  METAL-CATALYSTS ;  POROUS CARBON ;  IRON ;  NANOPARTICLES
语种: 英语
WOS记录号: WOS:000407540200034
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/149816
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.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:
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.
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