疏水中空纳米结构MxMn3-xO4±δ@Ce(La)Oy低温催化氧化OVOCs(H2O)过程及作用机理

低温催化氧化是一种处理具有高大气反应活性和高臭氧潜势含氧挥发性有机污染物（OVOCs）的优势控制方法，但环境H2O的存在易导致低温催化氧化材料活性降低、稳定性变差和失活等问题。项目旨在通过构建不同中空纳米结构疏水的稀土复合锰基尖晶石功能材料，以提升复杂环境介质中污染物催化反应活性和抗水性能。拟采用耦合调控相结构和界面相互作用行为策略，合成系列中空纳米球/片组装的疏水MxMn3-xO4±δ@Ce(La)Oy催化材料，实现环境H2O影响下的醛酮类OVOCs分子的选择吸附及高效催化氧化；并借助系列原位表征技术、同位素示踪技术及量化计算，探究催化剂上OVOCs污染物的吸(脱)附性、抗水性、稳定性以及反应过程中H2O分子行为特征；揭示其抗水过程及醛酮类分子中C-C、C-H、C=O键和O2分子O=O键活化、迁移及转化过程；阐明其低温催化氧化OVOCs（H2O）污染物的反应行为及抗水作用机理。

Low-temperature catalytic oxidation is an efficient technology to eliminate oxygenated volatile organic compounds (OVOCs) with high atmospheric reactivity and high ozone potential. However, the effect of H2O molecules is still a problem unsettled, which tend to cause the low catalytic activity, poor stability, and easy deactivation of catalysts for low-temperature catalytic oxidation technology. Therefore, the catalytic activity and water-resistance was improved by constructing rare earth oxide and manganese-based spinel composite functional materials with different hollow nanostructure. A series of hollow nanospheres/sheets assembled with hydrophobic MxMn3-xO4±δ@Ce(La)Oy catalytic materials were synthesized by using a coupling control phase structure and interface interaction methods. The aim is to achieve selective adsorption and efficient catalytic oxidation of aldehydes and ketones molecules in H2O and/or OVOCs pollutant on functional materials. The in-situ methods, isotope tracer technology, and quantitative calculations were used to study the adsorption (desorption) capacity, water-resistance, stability, and water molecular behavior of OVOCs (H2O) pollutants on catalysts, respectively. It reveals the water-resistance process, mechanism and the C-C, C-H, C=O and O=O chemical bond activation, migration and transformation in catalytic oxidation of aldehyde and ketone molecules, respectively. Finally, it clarifies the low-temperature catalytic oxidation process of OVOCs (H2O) and water-resistance mechanism of MxMn3-xO4±δ@Ce(La)Oy hollow nanostructured materials.