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Continuous heterogeneous hydrogenation of CO2-derived dimethyl carbonate to methanol over a Cu-based catalyst

机译:在Cu基催化剂上连续的非均相碳酸二碳酸二甲酯与甲醇的氢化

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Catalytic mild hydrogenation of carbonates synthesized from the CO2 captured by alcohols is of significant interest both conceptually and practically, which provides alternative approaches to the indirect hydrogenation of CO2 to methanol. However, the catalytic efficiency of the process of dimethyl carbonate (DMC) hydrogenation still remains unsatisfactory. Unprecedented gas-solid phase fix-bed catalyzed hydrogenation of DMC to methanol has been made. Herein, we address this issue with facile Cu/SiO2 catalysts, reaching complete conversion and highly selective formation of methanol (up to 80% yield) under mild conditions (503 K, 2.5 MPa), which is the highest yield that has been reported. Characterization results indicate that the copper dispersion and the synergetic effect between balanced Cu-0 and Cu+ sites are considered to play critical role in attaining high yield of methanol. The optimized Cu/SiO2 catalyst displayed excellent catalytic performance in the hydrogenation of diethyl carbonate (DEC) and di-n-propyl carbonate (DPC) as well, presenting a broad substrate scope. Moreover, the comparative catalytic activity (similar to 76% methanol yield) in the hydrogenation of DMC under solvent-free conditions shows promise for its scalable application in industry.
机译:从由醇捕获的CO2合成碳酸盐的轻度催化加氢是显著兴趣概念上和实用上,其提供替代方法的CO 2与甲醇的间接氢化的。然而,碳酸二甲酯(DMC)氢化的过程中的催化效率仍然不能令人满意。 DMC的甲醇前所未有气 - 固相固定床催化氢化已经取得进展。在此,我们解决这个问题与轻便的Cu / SiO2催化剂,达到完全转化且在温和的条件(503 K,2.5兆帕),其是已被报道的最高产率下的甲醇中高度选择性形成(高达80%收率)。鉴定结果表明,铜的分散性和平衡的Cu-0和Cu +站点之间的协同效应被认为是实现甲醇的高产起到至关重要的作用。优化的铜/二氧化硅催化剂在碳酸二乙酯(DEC)和二 - 正 - 丙基碳酸酯(DPC)的氢化中显示优异的催化性能,以及,呈现出广泛的底物范围。此外,比较催化活性的DMC下无溶剂条件示出了加氢(类似于76%甲醇的产率)保证在工业其可扩展的应用。

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