Discriminating Catalytically Active FeNx Species of Atomically Dispersed Fe-N-C Catalyst for Selective Oxidation of the C-H Bond

	Discriminating Catalytically Active FeNx Species of Atomically Dispersed Fe-N-C Catalyst for Selective Oxidation of the C-H Bond
	Liu, Wengang 1,2; Zhang, Leilei 1; Liu, Xin 1; Liu, Xiaoyan 1; Yang, Xiaofeng 1; Miao, Shu 1; Wang, Wentao 1; Wang, Aiqin 1; Zhang, Tao 1
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2017-08-09
卷号	139 期号:31 页码:10790-10798
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.
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Chemistry, Multidisciplinary
研究领域[WOS]	Chemistry
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
收录类别	SCI
语种	英语
WOS记录号	WOS:000407540200034
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/149806]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
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
推荐引用方式 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.