贵金属催化剂理性设计在选择性加氢反应中的研究进展

从多相催化的特征出发,综述了多相催化理性设计中典型调控理论和方法的研究进展。同时,以芳香硝基化合物及不饱和醛/酮选择性加氢反应为特征反应,从多相催化剂表面的电子效应、几何效应、界面效应和协同效应等角度进行了全面综述。指出了筛选合适的载体、合成特定尺寸形貌的活性中心、调控金属-载体强相互作用是开发更高效的多相选择性加氢催化剂的重要方向,调控金属-载体强相互作用,优化活性中心的电子效应、空间效应和界面效应,微调N=O及C=O不饱和键的吸附与活化,是实现高效选择性加氢催化体系的理论设计的重要手段。进一步优化氢气的活化裂解方式、活性氢的稳定与迁移,可抑制选择性加氢的副反应。

Research progress rational design of noble metal catalysts for selective hydrogenation

Based on the characteristics of heterogeneous catalysis,the research progress of typical regulatory theories and methods in the rational design of heterogeneous catalysis was reviewed.Meanwhile,from the perspectives of electronic effects,geometric effects,interfacial effects and synergetic effects,the relationship between surface structure of active centers and selective hydrogenation performance was reviewed comprehensively,with selective hydrogenation of aromatic nitro compounds and unsaturated aldehydes/ketones as a probe reaction.It was pointed out that selecting suitable supports,synthesizing metal active centers with specific size and morphology,and regulating the strong metal-support interaction were effective ways to regulate the performance of selective hydrogenation catalysts.The adsorption and activation of N=O and C=O could be precisely tuned by optimizing the electronic effect,spatial effect and interface effect of active center resulted from the strong metal-support interaction,which was important to the rational design of efficient selective hydrogenation catalysts.Further optimization of hydrogen activation cracking mode,stability and migration of active hydrogen could inhibit the side reaction of selective hydrogenation.