文献类型：期刊文献

英文题名：Kinetics Insights and Active Sites Discrimination of Pd-Catalyzed Selective Hydrogenation of Acetylene

作者：Cao, Yueqiang[1];Fu, Wenzhao[1];Sui, Zhijun[1];Duan, Xuezhi[1];Chen, De[2];Zhou, Xinggui[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2019

卷号：58

期号：5

起止页码：1888

外文期刊名：INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH

收录：;EI(收录号：20190506456264);WOS:【SCI-EXPANDED(收录号:WOS:000458348200011)】；

基金：This work was financially supported by the National Basic Research Program of China (973 Project, 2012CB720500), the Natural Science Foundation of China (21776077), the Shanghai Natural Science Foundation (17ZR1407300 and 17ZR1407500), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, the Shanghai Rising-Star Program (17QA1401200), the Open Project of State Key Laboratory of Chemical Engineering (SKLChe-15C03), the State Key Laboratory of Organic-Inorganic Composites (oic-201801007), and the Fundamental Research Funds for the Central Universities (222201718003). We thank Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterization.

语种：英文

外文关键词：Acetylene - Activation energy - Electronic properties - Binding energy - Kinetics - Catalyst activity - Particle size analysis - Hydrogenation - Particle size - Lighting

摘要：Catalysis is a kinetics behavior, and developing the kinetics-assisted discrimination of the active sites is an important yet challenging issue in the heterogeneous catalysis. Herein, we combine the multifaceted kinetics analysis with the model calculations to discriminate the dominant active sites in Pd-catalyzed semihydrogenation of acetylene. The size-insensitive activation energy of >= 3.1 nm sized Pd catalysts with similar electronic properties suggests that only one typed active site mainly dominates the acetylene hydrogenation. The results of model calculations, based on the specific cuboctahedron shape of Pd nanoparticles on CNT, indicate that the Pd(111) facet is dominant active sites for the reaction and the formation of C-4 byproduct, while the Pd corner site for the formation of ethane. Moreover, for the Pd particle size being smaller than 3.1 nm, the catalysts exhibit higher activation energy but higher TOF, due to their lower Pd-0 3d binding energy and higher pre-exponential factor, respectively.