Selective Conversion of Methane by Rh-1-Doped Aluminum Oxide Cluster Anions RhAl2O4-: A Comparison with the Reactivity of PtAl2O4-

doi:10.1021/acs.jpca.8b02483

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	Selective Conversion of Methane by Rh-1-Doped Aluminum Oxide Cluster Anions RhAl2O4-: A Comparison with the Reactivity of PtAl2O4-
	Li, Ya-Ke 1,2,3; Zhao, Yan-Xia 1,2; He, Sheng-Gui 1,2,3
刊名	JOURNAL OF PHYSICAL CHEMISTRY A
	2018-04-19
卷号	122 期号:15 页码:3950-3955
ISSN号	1089-5639
DOI	10.1021/acs.jpca.8b02483
英文摘要	Studying the elementary reactions of single-noble-metal-atom-doped species can give theoretical guidance for the design of related single-atom catalysis. Using a combination of mass spectrometry and density functional theory calculations, the reaction of RhAl2O4- with the most stable alkane molecule CH4 under thermal conditions has been studied. The methane tends to be converted into syngas (free H-2 and adsorbed CO) with activation of four C-H bonds. In sharp contrast, formaldehyde was generated in the previously reported reaction of PtAl2O4- with CH4. Density functional theory calculations show that the difference in reactivity between RhAl2O4- and PtAl2O4- is found to be due to a higher energy barrier of the third C-H bond activation for the Pt analogue. This work provides the first comparative study on the reactivity of single noble-metal atoms (Rh, Pt) on the same cluster support (Al2O4-) and can be helpful for rational design of single-atom catalysts for selective methane conversion.
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000430783700026
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/43253]
专题	中国科学院化学研究所
通讯作者	Zhao, Yan-Xia; He, Sheng-Gui
作者单位	1.Chinese Acad Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China 2.CAS Res Educ Ctr Excellence Mol Sci, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Li, Ya-Ke,Zhao, Yan-Xia,He, Sheng-Gui. Selective Conversion of Methane by Rh-1-Doped Aluminum Oxide Cluster Anions RhAl2O4-: A Comparison with the Reactivity of PtAl2O4-[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2018,122(15):3950-3955.
APA	Li, Ya-Ke,Zhao, Yan-Xia,&He, Sheng-Gui.(2018).Selective Conversion of Methane by Rh-1-Doped Aluminum Oxide Cluster Anions RhAl2O4-: A Comparison with the Reactivity of PtAl2O4-.JOURNAL OF PHYSICAL CHEMISTRY A,122(15),3950-3955.
MLA	Li, Ya-Ke,et al."Selective Conversion of Methane by Rh-1-Doped Aluminum Oxide Cluster Anions RhAl2O4-: A Comparison with the Reactivity of PtAl2O4-".JOURNAL OF PHYSICAL CHEMISTRY A 122.15(2018):3950-3955.