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课题组在介孔CeO2表面实现活性中心构筑并用于CO2加氢反应取得进展
发布时间:2023-06-06

采用湿法浸渍法在介孔Co/CeO2-δ催化剂上构建包括金属Co、表面氧空位和Co0-CeO2-δ界面结构的表面活性中心,表面活性中心可以通过Co物种的剂量来调节。金属CoCeO2-δ之间的相互作用能促进表面氧空位和Co0-CeO2-δ界面结构的形成,有利于抑制高温环境中Co物种的聚集和烧结。所制备的Co/CeO2-δ催化剂比单组分CoCeO2-δ催化剂具有更好的CO2加氢催化性能,这归因于Co0活性中心、表面氧空位和Co0-CeO2-δ界面结构之间的协同作用。因此,Co/CeO2-δ催化剂对反应物CO2H2分子具有较强的吸附和活化能力,提高了CO2加氢活性。在常压和400 °C下,Co负载量为12%Co/CeO2-δ催化剂上的CO2转化率和CH4选择性分别达到59.7%95.7%,并在9个循环中保持了良好的稳定性。

Guilin Zhou*, Shan Zhao, Fengqiong Xie, Shuang Chen, Hongmei Xie. Construction of surface active centers on the mesoporous Co/CeO2-δ catalysts for CO2 hydrogenation [J]. International Journal of Hydrogen Energy, 2023, 48(74): 28980–28997. https://doi.org/10.1016/j.ijhydene.2023.04.107

The surface active centers, which include metal Co, surface oxygen vacancies, and Co0-CeO2-δ interface structures, can be constructed on the mesoporous Co/CeO2-δ catalysts by wet impregnation method. And the surface active centers can be regulated by the Co species dosage. The interaction between the metal Co and CeO2-δ can promote surface oxygen vacancies and Co0-CeO2-δ interface structures to be formed and be conducive to inhibit the aggregation and sintering of Co species in high temperature environment. The prepared Co/CeO2-δ catalysts have better catalytic performances for CO2 hydrogenation than the single component Co and CeO2-δ catalysts, which can be attributed to the synergistic effect between Co0 active centers, surface oxygen vacancies, and Co0-CeO2-δ interface structures. Therefore, the Co/CeO2-δ catalysts have strong adsorption and activation ability for reactant CO2 and H2 molecules to improve the CO2 hydrogenation activity. At atmospheric pressure and 400 °C, the CO2 conversion and CH4 selectivity on the Co/CeO2-δ catalyst with Co loading of 12 % could reach 59.7 % and 95.7 %, respectively, and maintained good stability in 9 cycles for CO2 hydrogenation reaction.