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Kinetics-assisted identification and regulation of active sites for Pd-catalyzed propyne selective hydrogenation |
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| Authors: | Kelin Yan Yueqiang Cao Xiaohu Ge Yurou Li Jing Zhang Xueqing Gong Gang Qian Xinggui Zhou Xuezhi Duan |
| Affiliation: | 1. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, China
Contribution: Data curation (lead), Investigation (equal), Writing - original draft (equal);2. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, China;3. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, China Contribution: Data curation (supporting), Investigation (supporting);4. Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai, China Contribution: Data curation (supporting);5. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, China Contribution: Data curation (supporting) |
| Abstract: | Identification and regulation of active sites are significant for guiding the design and optimization of hydrogenation catalysts toward the target product but remain a great challenge. Herein, we demonstrate a kinetics-assisted identification method combined with theoretical calculations for identifying and further regulating the dominant active sites of Pd catalysts for propyne hydrogenation. Kinetics analysis and model calculations based on the cuboctahedron shape of Pd nanoparticles in the catalysts indicate the Pd(111) sites as the dominant active sites for the propyne conversion and propylene formation while the Pd(100) sites as those for the propane formation, which are further rationalized by theoretical calculations. Moreover, the Pd catalyst with electron-rich properties exhibits relatively higher activity and selectivity, guided by which the SiO2 support with abundant electron-donating hydroxyl groups is employed to increase the Pd electron density. Such electronic regulation for the Pd catalyst clearly enhances the selective hydrogenation of propyne. |
| Keywords: | active site electronic properties Pd catalysts Propyne hydrogenation structure sensitivity |