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Highly dispersed Pt nanoparticles confined within hierarchical pores of silicalite-1 zeolite via crystal transformation of supported Pt/S-1 catalyst for partial oxidation of methane to syngas
Affiliation:1. College of Chemistry & Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, PR China;2. Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, PR China;3. School of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng 252000, PR China;1. College of Chemistry & Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, PR China;2. Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, PR China;1. Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, United States;2. Chemical Sciences Division, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, CA 94720, United States;3. Department of Chemistry, Chonnam National University, 77 Yongbong-ro, Buk-gu, Gwangju 500-757, Republic of Korea;4. Department of Chemical Engineering, University of California, Berkeley, Berkeley, CA 94720, United States;1. Lodz University of Technology, Institute of General and Ecological Chemistry, Zeromskiego 116, 90-924 Lodz, Poland;2. UPMC Univ Paris 06, Laboratoire de Réactivité de Surface, Case 178, Site d’Ivry-Le Raphaël, 3 rue Galilée, 94200 Ivry sur Seine, France;3. CNRS-UMR 7197, Laboratoire de Réactivité de Surface, Case 178, Site d’Ivry-Le Raphaël, 3 rue Galilée, 94200 Ivry sur Seine, France;1. College of Environmental Science and Engineering, Taiyuan University of Technology, Jinzhong, 030600, Shanxi, PR China;2. Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, Taiyuan University of Technology, Taiyuan, 030024, Shanxi, PR China
Abstract:Highly dispersed Pt nanoparticles confined within hierarchical pores of silicalite-1 zeolite were prepared via crystal transformation of supported Pt/S-1 catalyst. Selective dissolution and external recrystallization in tetrapropylammonium hydroxide solution enabled metal nanoparticles to be encapsulated in zeolites. The abundant pore structures of as-prepared Pt@S-1 catalyst were obtained by properly controlling the time of desilication and recrystallization. The properties of Pt@S-1 catalyst with hierarchical pores were characterized by XRD, ICP, SEM, TEM/HRTEM, N2/Ar adsorption-desorption, CO adsorption, H2-TPR and TGA techniques. Compared with the traditional supported Pt/S-1 catalyst, Pt@S-1 catalyst exhibited excellent sintering resistance, owing to the restriction of the recrystallized shell. Further, abundant pore provided access to contact with the active components, the Pt@S-1 catalyst showed excellently catalytic performance. CH4 conversion and product selectivity were significantly improved. The out-standing catalytic performance was attributed to recrystallization of silica supported Pt. The strategy afforded enriched pore structure, improved the dispersion of active metal, and reduced the size of Pt nanoparticles. In addition, hierarchical pores of silicalite-1 zeolite supports also contributed to shorten the diffusion path of reactions.
Keywords:Partial oxidation of methane  Hierarchical pores of silicalite-1 zeolite  Crystal transformation  Pt nanoparticles
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