Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair
文献类型：期刊论文
| 作者 | Zhang, Tao1; An, Jinghua1,2; Wang, Yehong1; Lu, Jianmin1; Zhang, Jian1; Zhang, Zhixin1; Xu, Shutao1; Liu, Xiaoyan1; Gocyla, Martin3,4; Heggen, Marc3,4 |
| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 |
| 出版日期 | 2018-03-21 |
| 卷号 | 140期号:11页码:4172-4181 |
| ISSN号 | 0002-7863 |
| DOI | 10.1021/jacs.8b01742 |
| 文献子类 | Article |
| 英文摘要 | The interface of metal-oxide plays pivotal roles in catalytic reactions, but its catalytic function is still not clear. In this study, we report the high activity of nanostructured Ru/ceria (Ru-clusters/ceria) in the ethylene methoxycarbonylation (EMC) reaction in the absence of acid promoter. The catalyst offers 92% yield of MP with TOF of 8666 h(-1), which is about 2.5 times of homogeneous Pd catalyst (similar to 3500 h(-1)). The interfacial Lewis acid base pair [Ru-O-Ce-Vo], which consists of acidic Ce-Vo (oxygen vacancy) site and basic interfacial oxygen of Ru-O-Ce linkage, acts as active site for the dissociation of methanol and the subsequent transfer of hydrogen to the activated ethylene, which is the key step in acid-promoter-free EMC reaction. The combination of H-1 MAS NMR, pyridine-IR and DFT calculations reveals the hydrogen species derived from methanol contains Bronsted acidity. The EMC reaction mechanism under acid-promoter-free condition over Ru-clusters/ceria catalyst is discussed. |
| WOS关键词 | METAL-SUPPORT INTERACTIONS ; FINDING SADDLE-POINTS ; SOLID-STATE NMR ; CO OXIDATION ; CERIA CATALYSTS ; INFRARED-SPECTROSCOPY ; METHANOL SYNTHESIS ; IN-SITU ; PALLADIUM(II) COMPLEXES ; HETEROGENEOUS CATALYSIS |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:000428356000049 |
| 出版者 | AMER CHEMICAL SOC |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/168972]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Wang, Feng |
| 作者单位 | 1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Forschungszentrum Julich, Ernst Ruska Ctr Microscopy & Spect Electrons, D-52425 Julich, Germany 4.Forschungszentrum Julich, Peter Grunberg Inst, D-52425 Julich, Germany 5.Univ Trieste, INSTM, Ctr Excellence Nanostruct Mat CENMAT, Dept Chem & Pharmaceut Sci, Via L Giorgieri 1, I-34127 Trieste, Italy |
| 推荐引用方式 GB/T 7714 | Zhang, Tao,An, Jinghua,Wang, Yehong,et al. Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2018,140(11):4172-4181. |
| APA | Zhang, Tao.,An, Jinghua.,Wang, Yehong.,Lu, Jianmin.,Zhang, Jian.,...&Wang, Feng.(2018).Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,140(11),4172-4181. |
| MLA | Zhang, Tao,et al."Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 140.11(2018):4172-4181. |
入库方式： OAI收割
来源：大连化学物理研究所
浏览0
下载0
收藏0
其他版本
除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。