Synergistic Effects for Enhanced Catalysis in a Dual Single-Atom Catalyst | |
Fu, Junhong1; Dong, Jinhu2; Si, Rui4; Sun, Keju3; Zhang, Junying1; Li, Mingrun2; Yu, Nana1; Zhang, Bingsen4; Humphrey, Mark G.5; Fu, Qiang1,2; Huang, Jiahui1 | |
通讯作者 | Dong, Jinhu(jiahuihuang@dicp.ac.cn) ; Si, Rui(sirui@mail.sysu.edu.cn) ; Fu, Qiang(qfu@dicp.ac.cn) |
2021-02-19 | |
发表期刊 | ACS CATALYSIS
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ISSN | 2155-5435 |
卷号 | 11期号:4页码:1952-1961 |
摘要 | Synergistic effects have been discussed extensively in bimetallic heterogeneous catalysis, but it remains unclear how the effects function at the atomic scale. Here, we report a dual single-atom catalyst (DSAC) Ir1Mo1/TiO2 displaying much greater catalytic chemoselectivity (>96%, at 100% conversion) than comparable single-atom catalysts (SACs) Ir-1/TiO2 (38%, at 87% conversion) and Mo-1/TiO2 (no activity) for the hydrogenation of 4-nitrostyrene (4-NS) to 4-vinylaniline (4-VA). Activation of the TiO2-supported bimetallic carbonyl cluster Ir2Mo2(CO)(10)(eta(5)-C5H5) (2) in an Ar atmosphere affords the DSAC Ir1Mo1/TiO2. Characterization of the dual single-atom structure confirms that it consists of well-dispersed Ir single atoms (Ir-1) and Mo single atoms (Mo-1) on TiO2. Density functional theory studies reveal that Ir-1 sites effect H-2 activation while Mo-1 sites are responsible for 4-NS adsorption, with synergistic cooperation between the two sets of single atoms contributing to the better catalytic performance for the hydrogenation of 4-NS. This work provides a deep understanding of synergistic effects in dual single-atom catalysis. |
关键词 | bimetallic catalysis synergistic effects single-atom catalyst dual single-atom catalyst hydrogenation of nitrostyrene |
资助者 | National Natural Science Foundation of China ; Chinese Academy of Sciences ; National Key R&D Program of China ; Projects of International Cooperation and Exchanges NSFC ; International Postdoctoral Exchange Fellowship Program |
DOI | 10.1021/acscatal.0c05599 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | National Natural Science Foundation of China[21703235] ; National Natural Science Foundation of China[21688102] ; Chinese Academy of Sciences[XDB17000000] ; National Key R&D Program of China[2019YFC1905300] ; Projects of International Cooperation and Exchanges NSFC[21961142006] ; International Postdoctoral Exchange Fellowship Program |
WOS研究方向 | Chemistry |
WOS类目 | Chemistry, Physical |
WOS记录号 | WOS:000621598700007 |
出版者 | AMER CHEMICAL SOC |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/161217 |
专题 | 中国科学院金属研究所 |
通讯作者 | Dong, Jinhu; Si, Rui; Fu, Qiang |
作者单位 | 1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, iChEM, Dalian 116023, Peoples R China 3.Yanshan Univ, Key Lab Appl Chem, Coll Environm & Chem Engn, Qinhuangdao 066004, Hebei, Peoples R China 4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 5.Australian Natl Univ, Res Sch Chem, Canberra, ACT 2601, Australia |
推荐引用方式 GB/T 7714 | Fu, Junhong,Dong, Jinhu,Si, Rui,et al. Synergistic Effects for Enhanced Catalysis in a Dual Single-Atom Catalyst[J]. ACS CATALYSIS,2021,11(4):1952-1961. |
APA | Fu, Junhong.,Dong, Jinhu.,Si, Rui.,Sun, Keju.,Zhang, Junying.,...&Huang, Jiahui.(2021).Synergistic Effects for Enhanced Catalysis in a Dual Single-Atom Catalyst.ACS CATALYSIS,11(4),1952-1961. |
MLA | Fu, Junhong,et al."Synergistic Effects for Enhanced Catalysis in a Dual Single-Atom Catalyst".ACS CATALYSIS 11.4(2021):1952-1961. |
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