Hydrogen production from steam reforming of methanol over CuO/ZnO/Al2O3 catalysts: Catalytic performance and kinetic modeling

摘要/Abstract

摘要： A series of CuO/ZnO/Al₂O₃, CuO/ZnO/ZrO₂/Al₂O₃ and CuO/ZnO/CeO₂/Al₂O₃ catalysts were prepared by coprecipitation and characterized by N₂ adsorption, XRD, TPR, N₂O titration and HRTEM. The catalytic performances of these catalysts for the steam reforming of methanol were evaluated in a laboratory-scale fixed-bed reactor at 0.1 MPa and temperatures between 473 and 543 K. The results showed that the catalytic activity depended greatly on the catalyst reducibility and the specific surface area of Cu. An approximate linear correlation between the catalytic activity and the Cu surface area was found for all catalysts investigated in this study. Compared to CuO/ZnO/Al₂O₃, the ZrO₂-doped CuO/ZnO/Al₂O₃ exhibited higher activity and selectivity to CO, while the CeO₂-doped catalyst displayed lower activity and selectivity. Finally, an intrinsic kinetic study was carried out over a screened CuO/ZnO/CeO₂/Al₂O₃ catalyst in the absence of internal and external mass transfer effects. A good agreement was observed between the model-derived effluent concentrations of CO (CO₂) and the experimental data. The activation energies for the reactions of methanol-steam reforming, water-gas shift and methanol decomposition over CuO/ZnO/CeO₂/Al₂O₃ were 93.1, 85.1 and 116.5 kJ·mol^-1, respectively.

关键词: Steam reforming of methanol, CuO/ZnO/Al₂O₃, Dopants, Cu surface area, Kinetics

Abstract: A series of CuO/ZnO/Al₂O₃, CuO/ZnO/ZrO₂/Al₂O₃ and CuO/ZnO/CeO₂/Al₂O₃ catalysts were prepared by coprecipitation and characterized by N₂ adsorption, XRD, TPR, N₂O titration and HRTEM. The catalytic performances of these catalysts for the steam reforming of methanol were evaluated in a laboratory-scale fixed-bed reactor at 0.1 MPa and temperatures between 473 and 543 K. The results showed that the catalytic activity depended greatly on the catalyst reducibility and the specific surface area of Cu. An approximate linear correlation between the catalytic activity and the Cu surface area was found for all catalysts investigated in this study. Compared to CuO/ZnO/Al₂O₃, the ZrO₂-doped CuO/ZnO/Al₂O₃ exhibited higher activity and selectivity to CO, while the CeO₂-doped catalyst displayed lower activity and selectivity. Finally, an intrinsic kinetic study was carried out over a screened CuO/ZnO/CeO₂/Al₂O₃ catalyst in the absence of internal and external mass transfer effects. A good agreement was observed between the model-derived effluent concentrations of CO (CO₂) and the experimental data. The activation energies for the reactions of methanol-steam reforming, water-gas shift and methanol decomposition over CuO/ZnO/CeO₂/Al₂O₃ were 93.1, 85.1 and 116.5 kJ·mol^-1, respectively.

Key words: Steam reforming of methanol, CuO/ZnO/Al₂O₃, Dopants, Cu surface area, Kinetics

中图分类号:

10.1016/j.cjche.2016.02.006

YuWan, Zhiming Zhou, Zhenmin Cheng. Hydrogen production from steam reforming of methanol over CuO/ZnO/Al₂O₃ catalysts: Catalytic performance and kinetic modeling[J]. , 2016, 24(9): 1186-1194.

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Hydrogen production from steam reforming of methanol over CuO/ZnO/Al₂O₃ catalysts: Catalytic performance and kinetic modeling

Hydrogen production from steam reforming of methanol over CuO/ZnO/Al₂O₃ catalysts: Catalytic performance and kinetic modeling

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