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    ZnxCe2-yZryO4/SAPO-34双功能催化剂上CO2合成低碳烯烃

    CO2 synthesis of lower olefins over ZnxCe2-yZryO4/SAPO-34 bifunctional catalyst

    • 摘要: CO2加氢经接力催化可制备一系列燃料和化学品,是实现绿色化学的重要手段。通过溶胶凝胶法、共沉淀法和水热法制备了ZnxCe2-yZryO4金属氧化物,并与水热法制备的SAPO-34分子筛耦合组成ZnxCe2-yZryO4/SAPO-34双功能催化剂,研究其CO2加氢制备低碳烯烃的性能。本研究重点考察了不同制备方法对金属氧化物ZnxCe2-yZryO4的结构、表面氧空位浓度和加氢能力的变化情况及其对催化性能的影响。通过对比不同的温度、压力、耦合方式、质量比、空速等对催化性能的影响,获得最佳的反应条件。结果表明在350°C、4 MPa、6000 ml/g/h条件下溶胶凝胶法制备的催化剂表现出优异的催化性能,CO2转化率为12.44%,烃类产物中C2=-C4=选择性达到78.47%,总碳CO选择性仅为36.23%。基于此项研究为制备出高性能的CO2加氢制低碳烯烃的双功能催化剂提供了一定的理论见解。

       

      Abstract: Hydrogenation of CO2 via relay catalysis can prepare a range of fuels and chemicals and is an important means of achieving green chemistry. ZnxCe2-yZryO4 metal oxides were prepared by sol-gel, co-precipitation and hydrothermal methods and coupled with SAPO-34 molecular sieves prepared by hydrothermal method to form ZnxCe2-yZryO4/SAPO-34 bifunctional catalysts, and to study the performance of their CO2 hydrogenation for the preparation of lower olefins. This study focuses on the variation of the structure, surface oxygen vacancy concentration and hydrogenation capacity of the metal oxides ZnxCe2-yZryO4 by different preparation methods and their effects on the catalytic performance. The optimum reaction conditions were obtained by comparing the effects of different temperatures, pressures, coupling modes, mass ratios and air velocities on the catalytic performance. The results showed that the catalyst prepared by the sol-gel method at 350°C, 4 MPa, and 6000 ml/g/h exhibited excellent catalytic performance, with a CO2 conversion of 12.44%, a C2=-C4= selectivity of 78.47% in the hydrocarbon products, and a total carbon CO selectivity of only 36.23%. Based on this study, some theoretical insights have been provided for the preparation of high performance bifunctional catalysts for CO2 hydrogenation to lower olefins.

       

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