基于CO、CO2等小分子活化的纳米催化剂表界面结构调控

In heterogeneous catalysis, the activity, selectivity and stability of nanocatalysts are dependent on their surface/interface structures. This project, by selecting representative probe reactions (such as activation of small molecules like CO, CO2), plans to design and controllably synthesize nanocrystals with uniform size and shape, to obtain nanocatalysts with a variety of surface/interface structures, to investigate the adsorption, activation and desorption of involved chemical species on the surface/interface, and to unveil the corresponding physicochemical mechanisms in combination of theoretical simulation. Based on the above results, this project shall focus on those catalytic reactions of major industrial significance, conduct researches to elevate the catalyst performance, and specifically develop nanocatalysts with superior activity and stability. This project shall investigate the fundamental principles of the structure-property relationship of nanocatalysis, and specifically explore the applications of nanomaterials in important catalytic reactions.

催化剂的表界面结构直接决定了多相催化中催化剂的活性、选择性、稳定性。揭示催化剂表界面结构与催化性能之间的关系具有重要的科学意义。本课题旨在针对若干具有代表性的探针反应（如CO、CO2等小分子活化），进行单分散纳米材料的设计与调控合成，以获得具有不同表界面结构的纳米催化剂，探索反应物在此类催化剂表界面上的吸附、活化和产物的脱附方式，结合理论模拟，揭示催化反应的物理化学本质。并在此基础上，选择若干具有工业应用意义的催化反应，开展催化剂性能优化研究，有针对性地开发出具有高催化活性和选择性的纳米催化剂。本项目为探索催化表界面结构与性能之间的关联进行基础研究，又在纳米材料解决实际催化问题方面有针对性地开展应用研究，以期对高效纳米催化剂的实用化作出具有借鉴、参考意义的贡献。

本项目以表界面原子调控为手段，围绕二氧化碳、氧气、水、乙炔等小分子的活化反应，发展了若干纳米催化材料，探索了纳米催化剂的合成方法，研究了催化剂表界面结构和性能之间的构效关系，从原子、分子层面上认识了催化作用机理，顺利完成研究目标。发表论文32篇，其中包括Nat. Chem. 1篇、Nat. Catal. 1篇、Nat. Commun. 3篇、J. Am. Chem. Soc. 4篇、Angew. Chem. Int. Ed. 2篇、Adv. Mater. 3篇、Chem. Sci. 2篇等。