面向HCl催化氧化反应构建自限式氯化的二维纳米尖晶石催化剂的研究

针对非贵金属氧化物催化的HCl氧化反应，在充分分析其微观动力学复杂性及晶格内氯物种扩散的基础上，本课题以降低脱氯能垒、促进氧气解离吸附、消除氯物种的内扩散为核心思想，拟以金属组成丰富可调、稳定性高的尖晶石材料为研究对象，利用组成变化对金属位和氧空位电子性质的显著影响、二维限域带来的量子效应对表面金属位和氧空位数目及反应性的高度调控，以及对氯物种晶格内扩散的有效消除，构建以自限式氯化为特征的二维纳米尖晶石催化剂。本课题通过理论计算预测、高通量实验筛选及反应体系特定动力学研究多种手段密切结合，建立涵盖几个系列尖晶石材料的构效关系数据库，揭示量子效应对催化剂表面结构、物化性质及反应性能的调控机制，阐明尖晶石催化剂作用下的HCl催化氧化反应机理，最终获得高活性高稳定性尖晶石催化剂的优化制备技术及相关催化理论。本课题的开展，对于氯氧化反应的理论研究和广泛存在的工业应用都具有重要意义。

For the reaction of HCl catalytic oxidation to Cl2, the two-dimensional nano-spinel catalysts featured with self-limited chlorination will be developed in this project, based on the analysis of micro-kinetics and Cl species diffusion in lattice, aiming to reduce the desorption energy of Cl2, to eliminate the diffusion of C species, and to enhance the dissociation adsorption of O2. The effect of the spinel composition and the quantum effect aroused by the two-dimensional confinement on the metal and oxygen vacancy sites as well as the reactivity of catalysts will be investigated in detail. Trough theoretical calculations prediction, high-through experiments sieving, and special kinetics study, a structure-performance database of spinels including several types will be constructed, and the modulation mechanism of the quantum effect on the structure, property and performance of spinel catalysts will be revealed, and finally the key preparation technique of spinel catalysts with high activity and stability in HCl oxidation and the related catalytic theory will be obtained. Thus, the launch of this project is significant for both the theoretical research and industrial application of HCl catalytic oxidation reaction.