As global energy demand continues to increase and global climate change issues caused by greenhouse gas emissions gradually heat up, the effective conversion of carbon dioxide into high value-added methanol has become a key challenge in the energy and environmental fields. However, due to the chemical inertness of CO molecules, it is difficult to activate CO at low temperatures, resulting in extremely low conversion rates. Although increasing the reaction temperature is beneficial for the conversion of CO, there is also competition in the reverse water gas reaction, resulting in lower methanol selectivity. Therefore, developing efficient catalysts is the key to improving CO conversion rate and methanol selectivity. In this work, we used zirconium-based UIO-66 metal-organic framework as a precursor, replaced the original terephthalic acid ligand with thermally unstable aminoterephthalic acid, and supported Cu on the MOF precursor by equal volume impregnation method. After heat treatment, the Cu/ZrO-DM catalyst was prepared. The catalyst was compared with Cu/ZrO catalyst prepared by co-precipitation method, hydrothermal method and unmodified Cu/ZrO-D catalyst. The Cu/ZrO-DM catalyst exhibited the highest CO conversion and methanol selectivity in the hydrogenation reaction, reaching 13.95% and 90.78%, respectively. The main reason is attributed to the large specific surface area of the copper-based catalyst derived from MOF materials, the good dispersion of the active center and the strong interaction between Cu and the precursor. This work may provide a new perspective for the design and synthesis of related catalytic materials for efficient CO hydrogenation to methanol.

中文翻译：

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高度分散的活性位点和强金属-载体相互作用促进二氧化碳加氢生成甲醇

随着全球能源需求持续增加以及温室气体排放引发的全球气候变化问题逐渐升温，二氧化碳有效转化为高附加值甲醇已成为能源和环境领域的关键挑战。但由于CO分子的化学惰性，在低温下很难活化CO，导致转化率极低。虽然提高反应温度有利于CO的转化，但逆水煤气反应也存在竞争，导致甲醇选择性较低。因此，开发高效催化剂是提高CO转化率和甲醇选择性的关键。本工作以锆基UIO-66金属有机骨架为前驱体，用热不稳定的氨基对苯二甲酸替代原有的对苯二甲酸配体，通过等体积浸渍法将Cu负载在MOF前驱体上。热处理后，制备出Cu/ZrO-DM催化剂。将该催化剂与共沉淀法、水热法制备的Cu/ZrO催化剂以及未改性的Cu/ZrO-D催化剂进行了比较。 Cu/ZrO-DM催化剂在加氢反应中表现出最高的CO转化率和甲醇选择性，分别达到13.95%和90.78%。主要原因是MOF材料铜基催化剂具有较大的比表面积、良好的活性中心分散性以及Cu与前驱体之间的强相互作用。这项工作可能为CO高效加氢制甲醇相关催化材料的设计和合成提供新的视角。