期刊
SCIENCE CHINA-MATERIALS
卷 63, 期 9, 页码 1741-1749出版社
SCIENCE PRESS
DOI: 10.1007/s40843-020-1426-0
关键词
graphene; single-atom catalysts; acetylene hydrogenation; density functional theory
资金
- 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]
- Tsinghua National Laboratory for Information Science and Technology
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.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据