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首页> 外文期刊>ACS catalysis >Low-Temperature CO2 Hydrogenation to Liquid Products via a Heterogeneous Cascade Catalytic System
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Low-Temperature CO2 Hydrogenation to Liquid Products via a Heterogeneous Cascade Catalytic System

机译：通过多相级联催化系统将低温CO2加氢为液体产品

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Research described in this paper targeted a cascade system for the hydrogenation of CO2 to methanol via formic acid and/or formate intermediates, a reaction sequence that has been accomplished previously using homogeneous catalysts. On the basis of results for the hydrogenation of CO2, formic acid, and ethyl formate over a series of Cu- and Mo2C-based catalysts, we selected a Cu chromite catalyst for CO2 hydrogenation to the formate and a Cu/Mo2C catalyst to convert the formate to methanol. These catalysts worked cooperatively in the presence of ethanol, yielding a methanol turnover frequency of 4.7 x 10(-4) s(-1) at 135 degrees C, 10 bar of CO2, and 30 bar of H-2 in 1,4-dioxane. The performance for this Cu chromite:Cu/Mo2C cascade system surpassed the additive production of the individual catalysts by similar to 60%. The results also allowed an investigation of the reaction pathways. The hydrogenation of CO2 to formic acid appeared to be the rate-limiting step for most of the catalysts. This is not surprising given the thermodynamics for this reaction. Finally, the hydrogenation of CO2 to dimethyl ether was also demonstrated using a system consisting of the Cu/Mo2C catalyst to produce methanol from CO2 and HZSM-5 to produce dimethyl ether from methanol. The systems described in this paper are, to our knowledge, the first demonstrating cascade CO2 hydrogenation via heterogeneous catalysts.
机译：本文描述的研究目标是通过甲酸和/或甲酸酯中间体将CO2加氢成甲醇的级联系统，该反应序列以前已使用均相催化剂完成。根据一系列基于Cu和Mo2C的催化剂对CO2，甲酸和甲酸乙酯进行加氢的结果，我们选择了用于将CO2加氢成甲酸的亚铬酸铜催化剂和将Cu / Mo2C转化为Cu / Mo2C催化剂。甲酸酯制甲醇。这些催化剂在乙醇存在下协同工作，在135℃，10 bar的CO2和30 bar的H-2在1,4-甲醇中产生4.7 x 10（-4）s（-1）的甲醇转化频率。二恶烷。该亚铬酸铜：Cu / Mo2C级联系统的性能比单个催化剂的加成产量高出约60％。结果还允许研究反应途径。对于大多数催化剂而言，CO 2加氢成甲酸似乎是限速步骤。考虑到该反应的热力学，这不足为奇。最后，还证明了使用由Cu / Mo2C催化剂由CO2产生甲醇和HZSM-5由甲醇产生二甲醚组成的系统将CO2加氢成二甲醚。据我们所知，本文中描述的系统是第一个证明通过多相催化剂进行级联CO2加氢的系统。

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