Fuel ( IF 6.7 ) Pub Date : 2023-05-13 , DOI: 10.1016/j.fuel.2023.128647
Ren-You Huang , Thanh Truc Nguyen Hoang , Yu-An Hsueh , De-Hao Tsai
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In this study, a spray-drying approach is presented to develop (1) Cu-based metal–organic framework (Cu-MOF) supported on aluminum oxide nanoparticle cluster and (2) its derived Cu-ZnO/Al2O3 hybrid catalyst for combined (CO + CO2) hydrogenation to methanol. The results show superior high space time yield, 23.14 mmol gcat-1h−1, and selectivity to methanol (85%) were achievable under a moderate-pressure (30 bar) and relatively low-temperature (220 °C) operation. Incorporation of ZnO and Al2O3 (i.e., in the form of nanoparticle cluster) enhanced the dispersion and the redox ability of Cu in the MOF-derived catalyst, both of which were critical factors to the catalytic activity toward the combined hydrogenation of CO2 and CO to methanol. An optimal performance, in terms of the methanol yield, was achieved by using the catalyst with a Cu/Zn molar ratio of 2 and partially reduction by H2 at a relatively lower temperature (300 °C). The work demonstrates a new route for the design of MOF-derived catalyst by using an aerosol-assisted synthesis approach, showing promise for the catalysis of a variety of chemical reactions in the field of CO2 capture and utilization.
中文翻译:

使用气溶胶辅助的金属-有机骨架衍生杂化催化剂将 CO2 和 CO 联合加氢为甲醇
在这项研究中,提出了一种喷雾干燥方法来开发 (1) 负载在氧化铝纳米粒子簇上的铜基金属有机骨架 (Cu-MOF) 和 (2) 其衍生的 Cu-ZnO/Al 2 O 3杂化催化剂联合 (CO + CO 2 ) 加氢生成甲醇。结果表明,在中等压力 (30 bar) 和相对低温 (220 °C) 的操作下,可实现出色的高时空产率 23.14 mmol gcat -1 h -1和对甲醇的选择性 (85%)。ZnO和Al 2 O 3的掺入(即以纳米粒子簇的形式)增强了 Cu 在 MOF 衍生催化剂中的分散性和氧化还原能力,这两者都是对 CO 2 和 CO 联合加氢制甲醇的催化活性的关键因素。通过使用 Cu/Zn 摩尔比为 2 的催化剂并在相对较低的温度 (300 °C) 下通过 H 2进行部分还原,实现了就甲醇产率而言的最佳性能。该工作展示了一种使用气溶胶辅助合成方法设计 MOF 衍生催化剂的新路线,有望在 CO 2捕获和利用领域催化多种化学反应。