基于高分散型RuNi/CeCaO双功能材料的CO2捕集与原位催化转化技术研究

CO2捕集与转化对于推动CO2减排，实现“碳中和”以及绿色低碳循环经济具有重要意义。传统的CO2捕集与转化技术通常先进行CO2的捕集，再将吸附剂转移到另一个高温反应器中进行再生以及CO2的转化，降低能量利用效率的同时，对材料的抗磨损性能提出了严峻的挑战。因此，本项目提出制备同时具有吸附位点和催化位点的高分散型RuNi/CeCaO双功能材料，将捕集的CO2在同温、同压、同一个反应器中原位催化转化为附加值高的产品。首先通过一步溶胶凝胶法制备Ce掺杂的多孔CaO基高温吸附剂，探索结构导向剂柠檬酸的添加量和Ce的掺杂量对其吸附量与稳定性的影响。其次通过浸渍法制备高分散型RuNi/CeCaO双功能材料，并探究金属的种类、分散程度与空间分布对其加氢能力的影响。最后结合原位技术，监测吸附剂烧结与催化剂积碳的过程，探索活性中间物种的形成与演变，进一步指导高分散型双功能材料的制备。

CO2 capture and conversion is of great significance for reducing CO2 emissions, achieving "carbon neutrality" and a green, low-carbon circular economy. Conventional CO2 capture and conversion technology captures CO2 firstly, and then transfers the adsorbent to another high-temperature reactor for the adsorbent regeneration and sequential CO2 conversion. This process will not only reduce energy efficiency, but also raise serious challenges to the wear resistance of the materials. Herein, we propose the synthesis of highly dispersed RuNi/CeCaO dual-functional materials with both adsorption sites and catalytic sites, which can in-situ convert the captured CO2 into high value-added products at the same temperature, pressure, and in the same reactor. Firstly, Ce-doped CaO-based high-temperature adsorbents are prepared by the one-pot sol-gel method. The capacity and stability of carbon capture process are optimized through adjusting the addition amount of citric acid and Ce. Secondly, the highly dispersed RuNi/CeCaO dual-functional materials are prepared by the impregnation method. In addition, the influence of metal type, dispersion and spatial distribution on the in-situ catalytic hydrogenation capacity is studied. Finally, the in-situ characterization is conducted to monitor the process of adsorbent sintering and carbon deposition on the catalyst, explore the formation and evolution of active intermediate species, and further guide the preparation of highly dispersed dual-functional materials.