Water-Assisted Homolytic Dissociation of Propyne on a Reduced Ceria Surface

doi:10.1002/anie.201914271

CORC > 上海应用物理研究所 > 中国科学院上海应用物理研究所 > 中科院上海应用物理研究所2011-2017年

	Water-Assisted Homolytic Dissociation of Propyne on a Reduced Ceria Surface
	Zhong, JQ ; Han, ZK ; Werner, K ; Li, XY ; Gao, Y ; Shaikhutdinov, S ; Freund, HJ
刊名	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
	2020
卷号	59 期号:15 页码:6150-6154
关键词	CEO2 HYDROGENATION OXIDE METHYLACETYLENE ADSORPTION CHEMISTRY CATALYSIS RH(111) SPECTRA FILMS
ISSN号	1433-7851
DOI	10.1002/anie.201914271
文献子类	期刊论文
英文摘要	The emergence of ceria (CeO2) as an efficient catalyst for the selective hydrogenation of alkynes has attracted great attention. Intensive research effort has been devoted to understanding the underlying catalytic mechanism, in particular the H-2-CeO2 interaction. Herein, we show that the adsorption of propyne (C3H4) on ceria, another key aspect in the hydrogenation of propyne to propene, strongly depends on the degree of reduction of the ceria surface and hydroxylation of the surface, as well as the presence of water. The dissociation of propyne and the formation of methylacetylide (CH3CC-) have been identified through the combination of infrared reflection absorption spectroscopy (IRAS) and DFT calculations. We demonstrate that propyne undergoes heterolytic dissociation on the reduced ceria surface by forming a methylacetylide ion on the oxygen vacancy site and transferring a proton to the nearby oxygen site (OH group), while a water molecule that competes with the chemisorbed methylacetylide at the vacancy site assists the homolytic dissociation pathway by rebounding the methylacetylide to the nearby oxygen site.
语种	英语
内容类型	期刊论文
源URL	[http://ir.sinap.ac.cn/handle/331007/33269]
专题	上海应用物理研究所_中科院上海应用物理研究所2011-2017年
作者单位	1.Max Planck Gesell, Dept Chem Phys, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany 2.Max Planck Gesell, Fritz Haber Inst, Theory Dept, Faradayweg 4-6, D-14195 Berlin, Germany 3.Chinese Acad Sci, Shanghai Inst Appl Phys, Div Interfacial Water, Shanghai 201800, Peoples R China 4.Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China 5.Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Lab, Shanghai 201210, Peoples R China
推荐引用方式 GB/T 7714	Zhong, JQ,Han, ZK,Werner, K,et al. Water-Assisted Homolytic Dissociation of Propyne on a Reduced Ceria Surface[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020,59(15):6150-6154.
APA	Zhong, JQ.,Han, ZK.,Werner, K.,Li, XY.,Gao, Y.,...&Freund, HJ.(2020).Water-Assisted Homolytic Dissociation of Propyne on a Reduced Ceria Surface.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,59(15),6150-6154.
MLA	Zhong, JQ,et al."Water-Assisted Homolytic Dissociation of Propyne on a Reduced Ceria Surface".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 59.15(2020):6150-6154.