Structural elucidation of supported Rh complexes derived from RhCl (PPh3)(3) immobilized on surface-functionalized SBA-15 and their catalytic performance for C-heteroatom (S, O) bond formation

doi:10.1016/j.jcat.2018.06.012

	Structural elucidation of supported Rh complexes derived from RhCl (PPh3)(3) immobilized on surface-functionalized SBA-15 and their catalytic performance for C-heteroatom (S, O) bond formation
	Yang, Yong 1,2; Chang, Ji Wong 2,4; Rioux, Robert M.2,3
刊名	JOURNAL OF CATALYSIS
	2018-09-01
卷号	365 页码:43-54
关键词	Rhodium Wilkinson's catalyst Surface organometallic catalyst Nuclear magnetic resonance Extended X-ray absorption spectroscopy Hydrothiolation Hydrosulfonation Stereoselectivity
ISSN号	0021-9517
DOI	10.1016/j.jcat.2018.06.012
英文摘要	The local structures of rhodium complexes derived from the immobilization of Wilkinson's complex, RhCI (PPh3)(3), on SBA-15 silica functionalized with primary-amine, secondary-amine, or diphenylphosphine groups within the mesoporous channels were characterized by a series of techniques including XRD, HR-TEM, multinuclear ((13)c/(29)si/P-31) solid-state NMR, 2D P-31{H-1) HETCOR NMR, XPS, and Rh K-edge EXAFS. Immobilization of RhCI(PPh3)(3) through covalent bond formation with different functional groups grafted to the silica surface lead to variations in the local structure of the Rh center that has important implications for catalysis. The immobilized Rh complexes demonstrated high activity for the addition of alkynes with thiols (hydrothiolation) or sulfonic acids (hydrosulfonation) with excellent regio- and stereoselectivity under mild reaction conditions. This work demonstrates the elucidation of the local structure of the immobilized Rh complexes requires a complimentary multi-technique characterization approach that probes both the metal center itself and surrounding ligands. (C) 2018 Elsevier Inc. All rights reserved.
资助项目	Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Sciences Program[DE-SC0016192] ; DOE Office of Science[DE-AC02-06CH11357] ; Qingdao Institute of Bioenergy and Bioprocess Technology (QIBEBT), Chinese Academy of Sciences[Y6710619KL]
WOS关键词	RHODIUM HYDROGENATION CATALYSTS ; ANTI-MARKOVNIKOV ADDITION ; TERMINAL ALKYNES ; WILKINSONS CATALYST ; VINYL SULFIDES ; INTERMOLECULAR HYDROAMINATION ; SOLID-STATE ; ORGANOMETALLIC CHEMISTRY ; CARBON NANOTUBES ; TRANS ADDITION
WOS研究方向	Chemistry ; Engineering
语种	英语
出版者	ACADEMIC PRESS INC ELSEVIER SCIENCE
WOS记录号	WOS:000442976400007
资助机构	Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Sciences Program ; DOE Office of Science ; Qingdao Institute of Bioenergy and Bioprocess Technology (QIBEBT), Chinese Academy of Sciences
内容类型	期刊论文
源URL	[http://ir.qibebt.ac.cn/handle/337004/11881]
专题	中国科学院青岛生物能源与过程研究所
通讯作者	Yang, Yong; Rioux, Robert M.
作者单位	1.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Key CAS Biobased Mat Lab, Qingdao 266101, Peoples R China 2.Penn State Univ, Dept Chem Engn, University Pk, PA 16802 USA 3.Penn State Univ, Dept Chem, University Pk, PA 16802 USA 4.Kumoh Natl Inst Technol, Dept Chem Engn, Gumi Si 39177, Kyeongsangbuk D, South Korea
推荐引用方式 GB/T 7714	Yang, Yong,Chang, Ji Wong,Rioux, Robert M.. Structural elucidation of supported Rh complexes derived from RhCl (PPh3)(3) immobilized on surface-functionalized SBA-15 and their catalytic performance for C-heteroatom (S, O) bond formation[J]. JOURNAL OF CATALYSIS,2018,365:43-54.
APA	Yang, Yong,Chang, Ji Wong,&Rioux, Robert M..(2018).Structural elucidation of supported Rh complexes derived from RhCl (PPh3)(3) immobilized on surface-functionalized SBA-15 and their catalytic performance for C-heteroatom (S, O) bond formation.JOURNAL OF CATALYSIS,365,43-54.
MLA	Yang, Yong,et al."Structural elucidation of supported Rh complexes derived from RhCl (PPh3)(3) immobilized on surface-functionalized SBA-15 and their catalytic performance for C-heteroatom (S, O) bond formation".JOURNAL OF CATALYSIS 365(2018):43-54.