Pt Single Atoms and Nanosized Clusters as Catalytic Reaction Platforms for Selective Hydrogenation Applications

被引:6
作者
Xu, Enze [1 ]
Feng, Haisong [1 ]
Wang, Lei [1 ]
Zhang, Yuanjing [1 ]
Liu, Kelong [1 ]
Cui, Shuai [1 ]
Meng, Hao [1 ]
Wang, Guirong [1 ]
Yang, Yusen [1 ]
机构
[1] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
single atom; nanosized cluster; selective hydrogenation; unsaturated aldehydes; structure-selectivitycorrelation; TOTAL-ENERGY CALCULATIONS; OXIDATION; ALLOY; FACET; NI;
D O I
10.1021/acsanm.3c02543
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
The exploitation and design of high-efficiency catalystshave attractedextensive attention in the selective regulation of hydrogenation reactions;however, it remains a tremendous challenge currently. Herein, we reporttwo kinds of nanosized Pt-based catalysts, including single-atom catalysts(SACs) and nanosized cluster catalysts (NCCs), anchored onto a CoAlO x support via the topotactic transformationof layered double hydroxides. The SAC (Pt-1/CoAlO x ) exhibits a >99% selectivity toward the hydrogenationof furfural (FAL) to furfuryl alcohol (FOL), while the NCC (Pt- n /CoAlO x ) showsa >99% selectivity for tetrahydrofurfuryl alcohol (THFOL) underamild reaction condition (room temperature and a 0.1 MPa pressure ofH(2)). Both in situ experiments and theoretical calculationsreveal that the aggregation state (single atom or nanosized cluster)of Pt atoms influences the adsorption configuration of FAL, in whichthe adsorption of C O occurs on Pt single atoms over Pt-1/CoAlO x and the adsorption ofboth C C and C O occurs on continuous Pt atoms overPt( n )/CoAlO x . The structure-selectivity relationship substantiates thatmetal ensemble size has an important effect on the adsorption structureof the reaction substrate and thus results in the different selectivityof the hydrogenation reaction.
引用
收藏
页码:14991 / 15001
页数:11
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