Abstract

Cu/ZnO/CeO₂ nanocomposite was supported on metal organic framework (MOF-5) to enhance active sites dispersion and control the nanoparticles agglomeration during synthesis through strong metal-support interactions. The incorporation of MOF-5 alleviated the obstacle facing the commercial ternary Cu/ZnO/Al₂O₃ regarding low surface area due to nanoparticles agglomeration. In addition, Cu/ZnO/CeO₂@MOF-5 gave higher methanol selectivity than the commercial catalyst which can be accounted for by the interfacial sites generated between MOF-5 and Cu/ZnO which favour methanol synthesis over carbon monoxide through regulating the intermediates bonding energies. CeO₂ as support for Cu/ZnO nanoparticles was also compared with commercial support and showed to have led to smaller particle size and superior dispersion of Cu active sites as well. Cu/ZnO/CeO₂@MOF-5 resulted in methanol STY of 23.3 mg g_cat h⁻¹ and selectivity of 79% at mild reaction temperature (260 °C) and pressure (10 bar). Two different MOFs including cerium based MOF and ZIF-8 demonstrated inferior performance compared to MOF-5.

Graphical Abstract

中文翻译：

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MOF-5 负载的 Cu/ZnO/CeO2 作为 CO2 加氢制甲醇的新型催化剂：CeO2 和 MOF-5 对活性位点影响的机理研究

摘要

Cu/ZnO/CeO ₂纳米复合材料负载在金属有机框架(MOF-5)上，通过强金属-载体相互作用增强活性位点分散并控制合成过程中纳米颗粒的团聚。MOF-5的加入缓解了商业三元Cu/ZnO/Al ₂ O ₃由于纳米粒子团聚而面临的低表面积问题。此外，Cu/ZnO/CeO ₂ @MOF-5比商业催化剂具有更高的甲醇选择性，这可以通过MOF-5和Cu/ZnO之间产生的界面位点来解释，该界面位点通过调节中间体有利于甲醇合成而不是一氧化碳键合能。作为 Cu/ZnO 纳米颗粒载体的CeO ₂也与商业载体进行了比较，结果表明 CeO 2 可以实现更小的粒径和更好的 Cu 活性位点分散性。Cu/ZnO/CeO ₂ @MOF-5在温和的反应温度（260℃）和压力（10巴）下产生23.3mg g _cat h ^{-1的甲醇STY和79%的选择性。}与 MOF-5 相比，两种不同的 MOF（包括基于铈的 MOF 和 ZIF-8）表现出较差的性能。

图形概要