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Cu/HMOR催化二甲醚羰基化合成乙酸甲酯: 催化剂制备方法的影响 (cited: 2)

Synthesis of Methyl Acetate by Dimethyl Ether Carbonylation over Cu/HMOR: Effect of Catalyst Preparation Method (cited: 2)

  • 摘要: 采用氨蒸发法、尿素水解法、离子交换法及浸渍法制备HMOR负载的Cu催化剂, 考察其催化二甲醚(DME)羰基化合成乙酸甲酯(MA)性能. 结果表明离子交换法制得Cu/HMOR催化剂在Cu的金属中心和酸性分子筛载体的共同作用下具有较好催化反应活性. 在210 oC、1.5 MPa、空速4883 h-1,DME转化率为95.3%,MA选择性为94.9%. 对催化剂进行N2物理吸附、X射线衍射、NH3程序升温脱附和CO程序升温脱附等表征发现,离子交换法制得Cu/HMOR催化剂具有较高比表面、大量弱酸及一定中强酸、适中的CO吸附强度,提高了CO插入DME羰基化反应活性.

     

    Abstract: Dimethyl ether carbonylation to methyl acetate was comparatively investigated over mor-denite supported copper (Cu/HMOR) catalysts prepared by different methods including evaporation, urea hydrolysis, incipient wetness impregnation and ion-exchange. The resultsshowed that Cu/HMOR prepared via iron-exchange method exhibited the highest catalytic activity due to the synergistic effect of active-site metal and acidic molecular sieve support. Conversion of 95.3% and methyl acetate selectivity of 94.9% were achieved under conditions of 210 oC, 1.5 MPa, and GSHV of 4883 h-1. The catalysts were characterized by nitrogen absorption, X-ray diffraction, NH3 temperature program desorption, and CO temperature program desorption techniques. It was found that Cu/HMOR prepared by ion-exchange method possessed high surface area, moderate strong acid centers, and CO adsorption cen-ters, which improved catalytic performance for the reaction of CO insertion to dimethyl ether.

     

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