铜基催化剂表面结构对于催化二氧化碳与含氮化合物反应的性能调控研究

The direct reaction between nitrogen-containing compounds and CO2 will play a vital role in the future energy and environmental fields. In this project, we will take advantage of synchrotron radiation-based techniques to investigate the control over the fine structures of copper-based nanomaterials and their structure-property relationship in CO2 conversion reactions, which will provide fundamentals for the design of copper-based nanomaterials towards direct reaction between nitrogen-containing compounds and CO2. Specifically, we will employ inorganic synthetic methods to control the structures of copper-based nanocrystals at atomic level. Leveraging these ideal model systems, we will investigate the effects of surface structures (including compositions and atomic arrangements) on catalytic activity and selectivity, in efforts to establish the structure-property relationship between catalyst surface structures and catalytic activities. The focus of research will include: (1) atomic-level control and X-ray absorption fine structure characterization for the surface structures of copper-based catalysts; (2) in-situ X-ray absorption spectroscopy and infrared spectroscopy characterizations for revealing the adsorption and activation process of CO2 and nitrogen-containing compounds; (3) establishment of structure-property relationship in the reactions between CO2 and nitrogen-containing compounds.

利用含氮化合物与二氧化碳反应来进行二氧化碳转化，在未来的催化领域中将起到重要作用。在本项目中，我们将基于几种同步辐射表征技术，研究相关转化体系的铜基催化剂精细结构控制及其构效关系，为针对含氮化合物与二氧化碳直接反应的催化剂设计提供理论基础。具体地，我们将利用无机可控合成方法，精准控制催化剂的表面精细结构，构建原子级别结构可控的铜基金属纳米催化剂；基于该理想材料模型，进一步探究其表面结构（包括原子排列方式和组分）对催化活性及选择性的具体影响，从而系统地建立催化剂表面结构与催化活性的构效关系。研究重点主要包括：（1）铜基催化剂表面结构的原子级别调控和X射线吸收精细结构表征；（2）二氧化碳分子和含氮化合物在催化剂表面的吸附活化状态的原位X射线吸收谱和红外光谱分析；（3）反应过程构-效关系的建立。

开发新型二氧化碳转化体系，在碳平衡领域中有巨大的潜力。在本项目中，我们重点基于原位近常压光电子能谱、原位红外光谱、原位X射线吸收谱，研究催化过程中的铜基催化剂精细结构控制及其构效关系，为针对二氧化碳催化转化催化剂设计提供理论基础。具体地：（1）项目团队利用无机可控合成方法，构建了原子级别结构可控且无未配位杂散N原子的单原子纳米催化剂，即二氧化碳催化剂表面结构的原子级别调控和X射线吸收精细结构表征；（2）分别开展碳氮两部分原料（二氧化碳分子/含氮原料）在催化剂表面的吸附活化状态的原位X射线吸收谱和红外光谱分析；（3）针对反应过程催化剂结构动态演化过程，基于原位X射线吸收精细结构分析开展二氧化碳催化转化过程中的构效关系建立。