CO2光催化转化催化剂表面性质可控调变及催化性能增强机理

CO2 photocatalytical conversion by using solar light has attracted a great of attentions, due to its potential in reducing CO2 emissions to meet the global environmental demands. Mesoporous metal oxide catalysts have been reported to be promising for CO2 photocatalytic conversion, due to their special porous structures and high surface areas. However, the activity of the mesoporous metal oxide catalysts to CO2 photocatalytical conversion is still very low. Surface properties, including surface acidity and alkalinity, surface defects and surface groups, of the catalysts are key factors affecting the CO2 photocatalytic conversion activity. Previously, we developed a cold plasma method, which is simple and green, for tuning surface properties of materials. In the present proposed work, we will enhance the activity of the mesoporous metal oxide catalysts to CO2 photocatalytic conversion through controllable tuning on their surface properties by using the cold plasma method at room temperature. An in-situ observation system will be constructed in experiments. By using the in-situ observation system as well as theoretical calculations, we will study the reasons for the enhanced performace of the mesoporous metal oxide catalysts in CO2 photocatalytic conversion, and explore the mechanism of CO2 photocatalytic conversion on the mesoporous metal oxide catalysts. It is believed that the present proposed work will be great helpful for achieving a controllable and targeted preparation of the catalysts with high activity to CO2 photocatalytic conversion.

CO2光催化转化是极具吸引力的CO2减排方式。具有特殊孔道结构和较大比表面积的介孔金属氧化物催化剂在CO2光催化转化中展现出良好的应用前景，但其反应效率仍然较低。催化剂表面酸碱性、缺陷位、基团等表面性质是影响CO2光催化转化效率的关键。冷等离子体法是我们在前期研究中开发的一种简单、绿色的材料表面改性方法。在本申请项目中，我们拟利用冷等离子体法实现室温条件下对介孔金属氧化物催化剂表面性质的可控调变，以提高其CO2光催化转化效率。通过在实验中建立原位在线监测系统，并结合理论计算，研究冷等离子体改性介孔金属氧化物催化剂上CO2光催化转化效率提高的原因，解析冷等离子体改性介孔金属氧化物催化剂上CO2光催化转化反应机理。最终实现以表面性质调变为导向的高效CO2光催化转化催化剂的可控定向制备。

针对CO2光催化转化效率低的问题，通过本项目实施，我们对介孔Al2O3、In2O3等催化剂表面性质进行可控调变，显著提高了光催化CO2转化效率；我们建立了冷等离子体操作条件、催化剂表面性质、催化性能间的定量关系，系统阐述了催化剂表面性质影响催化剂与CO2间的电子传递特性进而影响CO2吸附与转化的机制。研究成果为实现高效CO2转化催化剂的可控定制提供了强有力的实验和理论支撑。利用上述研究成果，在J. Am. Chem. Soc.、Catal. Sci. Technol.、Appl. Catal. B、Nano Res.等化学与化工重要期刊发表第一作者/通讯作者SCI论文7篇，并有1篇论文被选为Front Cover。