原位动态高分辨电子显微镜研究CO2加氢制甲醇模型催化剂：缺陷调控催化剂表界面结构及反应特性

针对CO2加氢制甲醇反应性能严重依赖于催化剂的缺陷，申请者基于缺陷调控关键物种交互作用原理，拟通过等离子体技术调控TiO2(001)纳米片缺陷、原子层沉积法负载Cu和CeOx，构建新型高效Cu/CeOx/TiO2纳米片模型催化剂。利用原位聚光镜球差校正扫描透射电子显微镜结合常规原位表征技术对催化剂表界面结构、反应特性进行原位、动态、高时空分辨的研究，多尺度揭示反应条件下铈、钛、氧空位、铜等关键物种间的交互作用机制，实现反应条件下关键物种快速协同转化迁移，结合反应性能获得催化剂表界面活性位的微观结构，阐明CO2活化与定向转化机制，最终基于缺陷化学从原子尺度提出CO2高效制甲醇催化剂的构建规律。研究成果将深化缺陷化学，发展通过缺陷调控精准设计与构建催化剂表界面局域原子和电子结构的新方法；发展原位动态高时空分辨的表征新技术和新理论；同时还有助于缓解全球气候变暖和提供安全可行的可再生能源存储技术。

In view of the reaction performance of CO2 hydrogenation to methanol is heavily dependent on the catalyst defects, based on the principle that the defect regulates the interactions of key species, the plasma technology is used to regulate the surface defects of TiO2 (001) nanosheets, and ALD method is utilized to load Cu and CeOx in order to construct a new high-efficiency Cu/CeOx/TiO2 nano-sheet catalyst. The surface structures and reaction characteristics of model catalysts are intended to be studied with in-situ dynamic high spatial and temporal resolution characterization technique, in situ spherical aberration corrected scanning electron microscopy. The mechanism of migration, transformation and interaction between various defects and different Cu species will be revealed at atomic scale. The rules of defect-regulated catalyst surface-interface microstructure will be established. The precise design and construction rules of the local atomic and electronic structures on the surface will be acquired, and the microstructures of the active sites of the catalysts will be obtained. The mechanism of CO2 activation and directional conversion will be elucidated to achieve low-energy and high-efficiency conversion to methanol. The research results will deepen defect chemistry, develop new methods to precisely control the surface and interface microstructures of catalysts through defects, develop new techniques and theories of in-situ dynamic high spatial-temporal resolution characterization, and also contribute to mitigating global warming and providing safe and feasible renewable energy storage technologies.