Effective Ensemble of Pt Single Atoms and Clusters over the (Ni,Co)(OH)(2) Substrate Catalyzes Highly Selective, Efficient, and Stable Hydrogenation Reactions
文献类型：期刊论文
| 作者 | Zhu, Lihua1,4,5; Sun, Yilun7; Zhu, Huaze; Chai, Guoliang7; Yang, Zhiqing6; Shang, Congxiao4,5; Ye, Hengqiang6; Chen, Bing Hui3; Kroner, Anna2; Guo, Zhengxiao4,5 |
| 刊名 | ACS CATALYSIS
 |
| 出版日期 | 2022-06-22 |
| 页码 | 8104-8115 |
| ISSN号 | 2155-5435 |
| 关键词 | Pt single atoms and atomic clusters (SAACs) (Ni,Co)(OH)(2) nanoparticles hydrogenation reactions synergistic effect hydrogen spillover |
| DOI | 10.1021/acscatal.2c01901 |
| 通讯作者 | Zhu, Lihua(zhulihua@jxust.edu.cn) ; Chai, Guoliang(g.chai@fjirsm.ac.cn) ; Yang, Zhiqing(yangzq@imr.ac.cn) ; Guo, Zhengxiao(zxguo@hku.hk) |
| 英文摘要 | A Pt-Ni-Co catalyst was synthesized with Pt single atoms and atomic clusters (SAACs) dispersed over (Ni,Co)(OH)(2) nanoparticles on a carbon matrix, which leads to high catalytic activity, up to 100% conversion, and selectivity in the hydrogenation of nitroaromatics under moderate conditions (H-2 similar to 1.0 MPa and <= 40 degrees C). A synergistically coordinated ensemble effect of the Pt SAACs is identified with the strongly polarized Pt single atoms preferentially adsorbing the -NO2 and the Pt clusters adsorbing and homolytically dissociating H-2 molecules, and the H species then readily move to the adsorbed -NO2 group, overcoming a much reduced energy barrier on the (Ni,Co)(OH)(2), enhancing the reaction rate by ca. 50 times. The approach not only reveals the coordinated ensemble catalysis mechanism of SAACs but also provides a strategy of developing highly efficient and selective catalysts by fine tuning of the electronic microenvironment from single atoms to atomic clusters co-located over a multimetallic substrate. The demonstrated case for nitroarenes can be readily applied for other species containing -NO2 or other easily hydrogenated groups (such as C=C, C Z, and C=O). |
| 资助项目 | National Natural Science Foundation of China[22162012] ; National Natural Science Foundation of China[21703248] ; Youth Jinggang Scholars Program in Jiangxi Province[[2019]57] ; Program of Technology Innovation Talents of Ganzhou ; Research Fund Program of Key Laboratory of Fuel Cell Technology of Guangdong Province ; Guangdong Provincial Key RD Program[2020B0101370003] ; National Key Research and Development Program of China[2017YFA0700103] ; National Key Research and Development Program of China[2018YFA0704502] ; Horizon 2020 Research and Innovation Program[862296-SABYDOMA] ; HKU Start-Up Fund ; HK Scholars Program ; EU/RGC Research and Innovation Cooperation Co-Funding Mechanism[RGC: E-HKU704/19] |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| 出版者 | AMER CHEMICAL SOC |
| WOS记录号 | WOS:000819457800001 |
| 资助机构 | National Natural Science Foundation of China ; Youth Jinggang Scholars Program in Jiangxi Province ; Program of Technology Innovation Talents of Ganzhou ; Research Fund Program of Key Laboratory of Fuel Cell Technology of Guangdong Province ; Guangdong Provincial Key RD Program ; National Key Research and Development Program of China ; Horizon 2020 Research and Innovation Program ; HKU Start-Up Fund ; HK Scholars Program ; EU/RGC Research and Innovation Cooperation Co-Funding Mechanism |
| 源URL | [http://ir.imr.ac.cn/handle/321006/174807]  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Zhu, Lihua; Chai, Guoliang; Yang, Zhiqing; Guo, Zhengxiao |
| 作者单位 | 1.Jiangxi Univ Sci & Technol, Fac Mat Met & Chem, Coll Chem & Chem Engn, Ganzhou Jiang Xi 341000, Peoples R China 2.Diamond Light Source, Chilton OX11 0DE, Oxfordsshire, England 3.Xiamen Univ, Coll Chem & Chem Engn, Natl Engn Lab Green Prod Alcohols Ethers Esters, Dept Chem & Biochem Engn, Xiamen 361005, Peoples R China 4.Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China 5.Univ Hong Kong, HKU CAS Joint Lab New Mat, Hong Kong, Peoples R China 6.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 7.Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China |
| 推荐引用方式 GB/T 7714 | Zhu, Lihua,Sun, Yilun,Zhu, Huaze,et al. Effective Ensemble of Pt Single Atoms and Clusters over the (Ni,Co)(OH)(2) Substrate Catalyzes Highly Selective, Efficient, and Stable Hydrogenation Reactions[J]. ACS CATALYSIS,2022:8104-8115. |
| APA | Zhu, Lihua.,Sun, Yilun.,Zhu, Huaze.,Chai, Guoliang.,Yang, Zhiqing.,...&Guo, Zhengxiao.(2022).Effective Ensemble of Pt Single Atoms and Clusters over the (Ni,Co)(OH)(2) Substrate Catalyzes Highly Selective, Efficient, and Stable Hydrogenation Reactions.ACS CATALYSIS,8104-8115. |
| MLA | Zhu, Lihua,et al."Effective Ensemble of Pt Single Atoms and Clusters over the (Ni,Co)(OH)(2) Substrate Catalyzes Highly Selective, Efficient, and Stable Hydrogenation Reactions".ACS CATALYSIS (2022):8104-8115. |
入库方式： OAI收割
来源：金属研究所
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