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CO2 hydrogenation to methanol over Cu-ZnO-CeO2 catalyst: Reaction structure–activity relationship, optimizing Ce and Zn ratio, and kinetic study
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-12-01 , DOI: 10.1016/j.cej.2023.147783
Rajan Singh , Kaushik Kundu , Kamal K. Pant

The catalytic conversion of captured CO2 to MeOH is a possible solution to mitigate the rising CO2 emissions and to develop a carbon neutral society. The present study unveiled the effect of incorporating CeO2 to the precursor chemistry of Cu/ZnO catalytic system. The relation between the density of strong basic sites and H2 adsorption sites with catalytic activity is established. At 250 °C, 30 bar and 3000 mLgcat−1h−1, more than 106.7 gMeOH kgcat−1h−1 the MeOH STY is obtained for the CZCe-10 catalyst. Further, the reaction kinetics are performed for the best-screened catalyst, within the temperature 220 °C-310 °C, pressure 10 bar-30 bar, GHSV 1500–7500 mL gcat−1h−1 and H2/CO2 ratio 1:1 to 5:1 range. The literature reported single site and dual site kinetic models are applied to the experimental data, and the dual site reaction mechanism is found to be better based on model correlation’s error variances.

中文翻译:


Cu-ZnO-CeO2 催化剂上 CO2 加氢制甲醇:反应结构-活​​性关系、优化 Ce 和 Zn 比例以及动力学研究



将捕获的二氧化碳催化转化为甲醇是缓解二氧化碳排放量上升和发展碳中和社会的一种可能的解决方案。本研究揭示了 CeO2 对 Cu/ZnO 催化体系前驱体化学的影响。建立了强碱性位点密度和H2吸附位点与催化活性之间的关系。在 250 °C、30 bar 和 3000 mLgcat−1h−1 下,CZCe-10 催化剂获得超过 106.7 gMeOH kgcat−1h−1 的 MeOH STY。此外,在温度220°C-310°C、压力10bar-30bar、GHSV 1500–7500mL gcat−1h−1和H2/CO2比例1:1的条件下,对最佳筛选的催化剂进行反应动力学。至 5:1 范围。将文献报道的单位点和双位点动力学模型应用于实验数据,根据模型相关性的误差方差发现双位点反应机制更好。
更新日期:2023-12-01
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