Copper doped Ce/Zr oxides catalysts derived from from mixed-metal MOFs for thermal CO2 hydrogenation

Converting CO2 to methanol is a one of the most promising process to recycle CO2. However, the selectivity and the yield to methanol of this process are low. To maximize turnover per metal site, we desire structures where every or most metal sites are exposed on a surface. Metal-organic frameworks emerged as an attractive template to derive nanostructured metal oxide particles dispersed in a porous carbon matrix. In this work, we synthesized metal oxide-derived Cu-doped Ce/Zr mixed cluster in UiO-66 with various Ce/Zr metal ratios. The controlled pyrolysis helps to avoid sintering of the formed metal oxides, and we expect the Cu species to be well dispersed in the support structure. However, the structure of the materials has not yet elucidated. In order to draw a correlation between the catalytic performance and the structure, the characterization of Ce-Zr, Cu-Cu, Cu-Zr, and Cu-Ce interactions are crucially required.

将二氧化碳（CO₂）转化为甲醇是最具前景的二氧化碳循环利用工艺之一。然而，该工艺生成甲醇的选择性与产率均偏低。为最大化每个金属位点的周转数，我们期望获得几乎所有或绝大多数金属位点均暴露于表面的结构。金属有机框架（Metal-Organic Frameworks，MOFs）作为极具吸引力的模板，可用于制备分散于多孔碳基质中的纳米结构金属氧化物颗粒。在本研究中，我们合成了具有不同Ce/Zr金属比例的、由UiO-66衍生的铜掺杂Ce/Zr混合团簇金属氧化物。可控热解有助于避免生成的金属氧化物发生烧结，且我们预期铜物种可良好分散于载体结构中。然而，该材料的结构尚未得到阐明。为建立催化性能与材料结构之间的关联，对Ce-Zr、Cu-Cu、Cu-Zr以及Cu-Ce相互作用进行表征至关重要。