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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
2020
Source PublicationANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN1433-7851
Volume59Issue:15Pages:6150-6154
Subtype期刊论文
AbstractThe 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.
KeywordCEO2 HYDROGENATION OXIDE METHYLACETYLENE ADSORPTION CHEMISTRY CATALYSIS RH(111) SPECTRA FILMS
DOI10.1002/anie.201914271
Indexed BySCI ; EI
Language英语
Citation statistics
Cited Times:2[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/33269
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.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
Recommended Citation
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.
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