纳米催化剂选择性调控的理论基础

Nano catalysts play essential roles in both selective alkane oxidation and selective hydrogenation. However, in most cases, how to tailor the catalysts to achieve high selectivity is still far from being fully understood. In this project, we will concentrate on mechanisms for several important processes, including selective oxidation of propane or butane to oxygenates, and selective hydrogenation for unsaturated compound. Systematic theoretical studies will help us to resolve some of the most fundamental issues in nano catalysis: (i) the thermodynamics and kinetic factors to control the shape and size of nano materials; (ii) understanding the catalytic functions of different elements or different sites ; (iii) adsorption and conversion for the reactants, intermediates, products; (iv) the mechanistic picture of C-H, C=C or C=O bond forming and breaking. Combined with experiments, we will eluciate the molecular factors for catalytic selectivity, and ultimately provide the scientific backbone for the design of novel nano catalyst.

纳米催化剂在选择烷烃氧化和选择催化还原中均发挥着极其重要作用。如何理解反应的构效关系，提升对新催化材料的选控能力是一个重要的科学问题。本项目将深入探讨丙烷、丁烷的选择氧化以及不饱和化合物的选择加氢过程。通过理论模拟，认识影响纳米催化剂形貌和尺寸的热力学和动力学控制因素，弄清表面上不同元素和不同反应位在反应中所起的功能，系统考察表面活性物种的生成和转化机制，揭示C-H，C=C，C=O键在表面上形成和断裂的微观机制。结合实验，阐明"选择转化"的科学内涵，为新型纳米催化剂的理性设计提供科学依据。

项目负责人近期围绕纳米表界面形貌控制及其催化机理开展系统的理论研究。细致考察了CO在金属/金属氧化物界面上氧化过程，所提出的的活性中心和反应机理均得到了实验的验证。应用配位化学的概念深入研究了小分子对Pt、Pd等纳米晶形貌的控制机理，以及对催化加氢选择性的调控机制，提出了催化剂优化改性的新策略，真正做到了理论指导和预言实验。阐明表面乙二醇基在光助Pd单原子生成过程中重要作用，揭示了单原子Pd具有优异加氢活性的本质。近年来在Science、Nature Mater.、 Nature Comm.、ACS Catal.、Chem.Comm.等重要国际期刊发表16篇SCI论文，应邀做多次国际、国内会议邀请报告。