Gas-phase hydrogenation of maleic anhydride to γ-butyrolactone over CeO2-promoted Cu-ZnO catalysts
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摘要: 采用共沉淀法制备了不同CeO2含量的铜锌催化剂。通过X射线粉末衍射、N2物理吸附、氢气程序升温还原、N2O脉冲吸附、氢气脉冲吸附等技术表征了催化剂的结构、物化性质。用固定床连续流动反应器研究了催化剂对顺酐气相加氢合成γ-丁内酯催化性能。结果表明,引入CeO2可调变铜锌催化剂的晶粒大小、还原性能、Cu0比表面积、氢气吸附性能。当CeO2质量分数小于3%时,催化剂的Cu晶粒随CeO2含量的增加而减小,催化剂的Cu0比表面积和氢气吸附性能随CeO2含量的增加而增大;当CeO2质量分数大于3%时,催化剂的Cu0比表面积和氢气吸附性能随CeO2含量的增加而减小。CeO2质量分数在3%~5%的催化剂催化顺酐气相加氢反应具有较高的稳定性。Abstract: A series of CeO2 promoted Cu-ZnO catalysts with different CeO2 content were prepared by co-precipitation method and characterized by X-ray diffraction, N2 adsorption-desorption (BET), hydrogen temperature-programmed reduction, N2O chemisorption, and H2 chemisorption. Hydrogenation of maleic anhydride to γ-butyrolactone was conducted over these catalysts in a fixed-bed continuous-flow reactor. Addition of CeO2 not only influenced the catalyst structure significantly by decreasing the CuO particle size, increasing the BET surface area, and Cu0 active area, but also had a significant enhancements in both reducibility and H2 uptakes of the catalysts. Promotion of CeO2 resulted in proper structural and good reducibility, which significantly increased the activity and the stability. With 3%~5% of CeO2 , CeO2-promoted Cu-ZnO catalysts showed highest activity and stability for the titled reaction.
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Key words:
- Cu-ZnO catalysts /
- CeO2 /
- maleic acid /
- hydrogenation /
- γ-butyrolactone
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