Water-Assisted Homolytic Dissociation of Propyne on a Reduced Ceria Surface
文献类型：期刊论文
| 作者 | Zhong, JQ; Han, ZK; Werner, K; Li, XY; Gao, Y; Shaikhutdinov, S; Freund, HJ |
| 刊名 | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
 |
| 出版日期 | 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 |
| 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. |
入库方式： OAI收割
来源：上海应用物理研究所
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