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

Zhong, J., Han, Z.-K., Werner, K., Li, X., Gao, Y., Shaikhutdinov, S. K., et al. (2020). Water‐Assisted Homolytic Dissociation of Propyne on a Reduced Ceria Surface. Angewandte Chemie International Edition, 59(15), 6150-6154. doi:10.1002/anie.201914271.

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 Creators:
Zhong, JianQiang1, Author           
Han, Zhong-Kang2, 3, 4, Author           
Werner, Kristin1, Author           
Li, Xiao‐Yan4, Author
Gao, Yi4, 5, Author
Shaikhutdinov, Shamil K.1, Author           
Freund, Hans-Joachim1, Author           
Affiliations:
1Chemical Physics, Fritz Haber Institute, Max Planck Society, ou_24022              
2NOMAD, Fritz Haber Institute, Max Planck Society, ou_3253022              
3Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, 143026, Moscow, Russia, ou_persistent22              
4Division of Interfacial Water and Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, 201800, Shanghai, China, ou_persistent22              
5Zhangjiang Laboratory, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210, Shanghai, China, ou_persistent22              

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 Abstract: 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 H2–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.

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Language(s): eng - English
 Dates: 2019-12-152019-11-082020-02-192020-04-06
 Publication Status: Published in print
 Pages: 5
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.201914271
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Title: Angewandte Chemie International Edition
  Abbreviation : Angew. Chem., Int. Ed.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 5 Volume / Issue: 59 (15) Sequence Number: - Start / End Page: 6150 - 6154 Identifier: ISSN: 1433-7851
CoNE: https://pure.mpg.de/cone/journals/resource/1433-7851