SMFs-supported Pd nanocatalysts in selective acetylene hydrogenation: Pore structure-dependent deactivation mechanism

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (5): 717-725.

SMFs-supported Pd nanocatalysts in selective acetylene hydrogenation: Pore structure-dependent deactivation mechanism

Elaheh Esmaeili^a,b,c, Ali Morad Rashidi^c, Yadollah Mortazavi^b, Abbas Ali Khodadadi^b, Mehdi Rashidzadeh^c

a. Birjand University of Technology, Department of Chemical Engineering, P. O. Box 97175/569, Birjand, Iran;
b. Catalysis and Nanostructured Materials Research Laboratory, School of Chemical Engineering, University of Tehran, Tehran 14155/6619, Iran;
c. Research Institute of Petroleum Industry (RIPI), West Blvd. Azadi Sport Complex, P. O. Box: 14665 1998, Tehran, Iran

收稿日期:2013-01-16 修回日期:2013-03-10 出版日期:2013-09-20 发布日期:2013-09-30
通讯作者: Ali Morad Rashidi

SMFs-supported Pd nanocatalysts in selective acetylene hydrogenation: Pore structure-dependent deactivation mechanism

Elaheh Esmaeili^a,b,c, Ali Morad Rashidi^c, Yadollah Mortazavi^b, Abbas Ali Khodadadi^b, Mehdi Rashidzadeh^c

a. Birjand University of Technology, Department of Chemical Engineering, P. O. Box 97175/569, Birjand, Iran;
b. Catalysis and Nanostructured Materials Research Laboratory, School of Chemical Engineering, University of Tehran, Tehran 14155/6619, Iran;
c. Research Institute of Petroleum Industry (RIPI), West Blvd. Azadi Sport Complex, P. O. Box: 14665 1998, Tehran, Iran

Received:2013-01-16 Revised:2013-03-10 Online:2013-09-20 Published:2013-09-30

摘要/Abstract

摘要： In the present study, CNFs, ZnO and Al₂O₃ were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction. The examined supports were characterized by SEM, NH₃-TPD and N₂ adsorption-desorption isotherms to indicate their intrinsic characteristics. Furthermore, in order to understand the mechanism of deactivation, the resulted green oil was characterized using FTIR and SIM DIS. FTIR results confirmed the presence of more unsaturated constituents and then, more branched hydrocarbons formed upon the reaction over alumina-supported catalyst in comparison with the ones supported on CNFs and ZnO, which in turn, could block the pores mouths. Besides the limited hydrogen transfer, N₂ adsorption-desorption isotherms results supported that the lowest pore diameters of Al₂O₃/SMFs close to the surface led to fast deactivation, compared with the other catalysts, especially at higher temperatures.

关键词: selective hydrogenation, alloy formation, acidic site, pore structure, SMFs-supported Pd nanocatalysts

Abstract: In the present study, CNFs, ZnO and Al₂O₃ were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction. The examined supports were characterized by SEM, NH₃-TPD and N₂ adsorption-desorption isotherms to indicate their intrinsic characteristics. Furthermore, in order to understand the mechanism of deactivation, the resulted green oil was characterized using FTIR and SIM DIS. FTIR results confirmed the presence of more unsaturated constituents and then, more branched hydrocarbons formed upon the reaction over alumina-supported catalyst in comparison with the ones supported on CNFs and ZnO, which in turn, could block the pores mouths. Besides the limited hydrogen transfer, N₂ adsorption-desorption isotherms results supported that the lowest pore diameters of Al₂O₃/SMFs close to the surface led to fast deactivation, compared with the other catalysts, especially at higher temperatures.

Key words: selective hydrogenation, alloy formation, acidic site, pore structure, SMFs-supported Pd nanocatalysts

Elaheh Esmaeili, Ali Morad Rashidi, Yadollah Mortazavi, Abbas Ali Khodadadi, Mehdi Rashidzadeh. SMFs-supported Pd nanocatalysts in selective acetylene hydrogenation: Pore structure-dependent deactivation mechanism[J]. 能源化学(英文), 2013, 22(5): 717-725.

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SMFs-supported Pd nanocatalysts in selective acetylene hydrogenation: Pore structure-dependent deactivation mechanism

SMFs-supported Pd nanocatalysts in selective acetylene hydrogenation: Pore structure-dependent deactivation mechanism

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