Atomic-Dispersed Rh Enables Efficient Catalytic Nitrile Hydrogenation: Size Effect and Metal-Dependent Effect
文献类型：期刊论文
| 作者 | Chen, Jiawei2,3; Jiao, Yueyue4,5,6; Qin, Xuetao7; Cai, Xiangbin1,8; Wang, Maolin7; Diao, Jiangyong3; Wang, Linlin3; Li, Chengyu7; Ren, Pengju4,5; Wen, Xiaodong4,5 |
| 刊名 | ACS CATALYSIS
 |
| 出版日期 | 2023-06-08 |
| 页码 | 8354-8361 |
| 关键词 | nitriles hydrogenation Rh catalyst atomically dispersed amines |
| ISSN号 | 2155-5435 |
| DOI | 10.1021/acscatal.3c01562 |
| 通讯作者 | Xiao, Dequan(dxiao@newhaven.edu) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn) |
| 英文摘要 | Thehydrogenation of nitriles to amines, as an atom-economicalsynthetic route, has attracted wide attention in industrial production.Despite that some catalysts for nitrile hydrogenation have been investigatedin recent years, achieving high activity and selectivity in this processremains a major challenge. Here, we fabricated an atomically dispersedRh catalyst anchored on defect-rich nanodiamond-graphene (ND@G) viaa deposition-precipitation strategy (Rh-1/ND@G),which showed the highest activity (TOF = 2592 h(-1)) in the hydrogenation of benzonitrile reaction among all the knowncatalysts under mild reaction conditions (333 K, 0.6 MPa H-2), and delivered high selectivity (>99%) toward secondary amines.Significantly, we prepared the Rh-cluster catalyst (Rh- n /ND@G) and a series of atomically dispersed M-1 catalysts (M = Rh, Ru, Pd, Ir, and Pt) to understand thesize effect and metal-dependent effect in the hydrogenation of benzonitrile.Experimental and theoretical investigations revealed that the Rh-1/ND@G catalyst has higher selectivity toward dibenzylaminethan Rh- n /ND@G, as it is less likely toform benzylamine on the Rh-1 active sites. Meanwhile, thedifference of adsorption energies (as a catalyst descriptor) betweenbenzylideneimine and benzonitrile was used to understand the activityof benzonitrile hydrogenation influenced by the metal-dependent effectof M-1 catalysts. Modulating the size and metal-dependenteffects could lead to high catalytic performance, paving the way todesign efficient nitrile hydrogenation catalysts. |
| 资助项目 | National Key R&D Program of China[2022YFA1504500] ; National Key R&D Program of China[2022YFB4003100] ; National Key R&D Program of China[2021YFA1502802] ; National Natural Science Foundation of China[22072162] ; National Natural Science Foundation of China[92145301] ; National Natural Science Foundation of China[U21B2092] ; National Natural Science Foundation of China[21961160722] ; International Partnership Program of Chinese Academy of Sciences[172GJHZ2022028MI] ; Dalian National Lab for Clean Energy (DNL Cooperation Fund)[202001] ; China Petrochemical Corporation[420043-10] ; China Petroleum & Chemical Corporation[420043-2] ; Shenyang Young Talents Program[RC210435] ; Shenyang National Laboratory for Materials Science ; Research Grants Council of Hong Kong[16306818] ; Research Grants Council of Hong Kong[C6021-14E] ; Research Grants Council of Hong Kong[N_HKUST624/19] ; Sinopec China ; Shanghai Synchrotron Radiation Facility (SSRF) ; Tencent Foundation through the XPLORER PRIZE and New Cornerstone Investigator Program |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:001003411900001 |
| 出版者 | AMER CHEMICAL SOC |
| 资助机构 | National Key R&D Program of China ; National Natural Science Foundation of China ; International Partnership Program of Chinese Academy of Sciences ; Dalian National Lab for Clean Energy (DNL Cooperation Fund) ; China Petrochemical Corporation ; China Petroleum & Chemical Corporation ; Shenyang Young Talents Program ; Shenyang National Laboratory for Materials Science ; Research Grants Council of Hong Kong ; Sinopec China ; Shanghai Synchrotron Radiation Facility (SSRF) ; Tencent Foundation through the XPLORER PRIZE and New Cornerstone Investigator Program |
| 源URL | [http://ir.imr.ac.cn/handle/321006/178234]  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Xiao, Dequan; Liu, Hongyang; Ma, Ding |
| 作者单位 | 1.Hong Kong Univ Sci & Technol, Ctr Quantum Mat, Hong Kong 999077, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 4.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China 5.Synfuels China Co Ltd, Natl Energy Ctr Coal Clean Fuel, Beijing 100871, Peoples R China 6.Univ Chinese Acad Sci, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100049, Peoples R China 7.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, P, Beijing 100871, Peoples R China 8.Hong Kong Univ Sci & Technol, Dept Phys, Kowloon, P, Hong Kong 999077, Peoples R China 9.SINOPEC, Res Inst Petr Proc, Dept Chem & Chem Engn, Beijing 100083, Peoples R China 10.Univ New Haven, Ctr Integrat Mat Discovery, Dept Chem & Chem Engn, West Haven, CT 06516 USA |
| 推荐引用方式 GB/T 7714 | Chen, Jiawei,Jiao, Yueyue,Qin, Xuetao,et al. Atomic-Dispersed Rh Enables Efficient Catalytic Nitrile Hydrogenation: Size Effect and Metal-Dependent Effect[J]. ACS CATALYSIS,2023:8354-8361. |
| APA | Chen, Jiawei.,Jiao, Yueyue.,Qin, Xuetao.,Cai, Xiangbin.,Wang, Maolin.,...&Ma, Ding.(2023).Atomic-Dispersed Rh Enables Efficient Catalytic Nitrile Hydrogenation: Size Effect and Metal-Dependent Effect.ACS CATALYSIS,8354-8361. |
| MLA | Chen, Jiawei,et al."Atomic-Dispersed Rh Enables Efficient Catalytic Nitrile Hydrogenation: Size Effect and Metal-Dependent Effect".ACS CATALYSIS (2023):8354-8361. |
入库方式： OAI收割
来源：金属研究所
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