Selective hydrogenation of acetylene on graphene-supported non-noble metal single-atom catalysts

Zhuo, Hong-Ying1,2,3; Yu, Xiaohu4; Yu, Qi4; Xiao, Hai2,3; Zhang, Xin1; Li, Jun2,3,5

2020-07-17

10.1007/s40843-020-1426-0

Science China-Materials   影响因子和分区

2095-8226

2199-4501

Large-scale production of polyethylene in industry requires efficient elimination of the trace amount of acetylene impurity. Currently, zeolite adsorption or the conversion of acetylene to ethyleneviaselective semi-hydrogenation on Pd catalysts is the commonly used method. In this work, we investigate the reaction mechanisms of acetylene hydrogenation on defective graphene (DG) supported single-atom catalysts (SACs), M-1/SV-G and M-1/DV-G (M=Ni, Pd and Pt) using density functional theory (DFT), where SV-G and DV-G represent DG with single and double vacancies, respectively. It is shown that the metal single-atoms (SAs) as well as their different coordination numbers both affect the activity and selectivity of the hydrogenation process. M-1/DV-G provides better H(2)dissociation ability than M-1/SV-G, which accounts for the poor acetylene hydrogenation activity of M-1/SV-G. Based on the reaction barriers, Pt-1/DV-G and Ni-1/DV-G are better catalysts than other systems considered here, with Ni-1/DV-G exhibiting high selectivity for the semi-hydrogenation product of acetylene. These results provide insights for the design of highly selective and noble-metal-free SACs for acetylene hydrogenation on carbon materials.

graphene single-atom catalysts acetylene hydrogenation density functional theory

SCI ; EI

英语

通讯

National Natural Science Foundation of China[21573286][21173269][21576288][U1662104][21590792][91645203] ; Ministry of Science and Technology of China[2015AA034603] ; Specialized Research Fund for the Doctoral Program of Higher Education[20130007110003] ; Science Foundation of China University of Petroleum, Beijing[2462015YQ0304] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002]

Materials Science

Materials Science, Multidisciplinary

WOS:000552183800003

SCIENCE PRESS

20203108991097

Catalyst selectivity ; Density functional theory ; Precious metals ; Zeolites ; Acetylene ; Ethylene ; Hydrogenation ; Atoms ; Design for testability ; Lighting

Precious Metals:547.1 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

Web of Science

1.China Univ Petr, Coll Chem Engn, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
2.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
3.Tsinghua Univ, Key Lab Organ Optoelect & Mol Engn, Minist Educ, Beijing 100084, Peoples R China
4.Shaanxi Univ Technol, Shaanxi Key Lab Catalysis, Hanzhong 723000, Peoples R China
5.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

Zhuo, Hong-Ying,Yu, Xiaohu,Yu, Qi,et al. Selective hydrogenation of acetylene on graphene-supported non-noble metal single-atom catalysts[J]. Science China-Materials,2020,63(9):1741-1749.

Zhuo, Hong-Ying,Yu, Xiaohu,Yu, Qi,Xiao, Hai,Zhang, Xin,&Li, Jun.(2020).Selective hydrogenation of acetylene on graphene-supported non-noble metal single-atom catalysts.Science China-Materials,63(9),1741-1749.

Zhuo, Hong-Ying,et al."Selective hydrogenation of acetylene on graphene-supported non-noble metal single-atom catalysts".Science China-Materials 63.9(2020):1741-1749.