离子束二氧化碳电还原催化剂缺陷调控及其动态演化研究

电化学还原CO2被认为是解决CO2排放的理想方法之一，但仍面临转化效率和产物选择性等问题。近年来，电催化剂缺陷调控被广泛研究证明可有效提升其转化效率和选择性。但当前缺陷制备手段难以实现缺陷类型、浓度以及空间分布协同调控，同时对于在真实电化学工作条件下缺陷演变及其缺陷调控本质仍缺乏系统深入认知。离子束辐照作为一种可工业化的表面改性技术，具有能量剂量精确可控等特点，可以在材料中引入不同类型、浓度的缺陷从而精确调控材料的电子性质和催化活性。因此申请人拟通过离子束辐照方法实现过渡金属氧化物缺陷构筑，从缺陷种类、浓度、分布三个维度系统研究材料中缺陷与CO2还原反应活性以及选择性相关关系。在此材料制备基础上，进一步通过原位电化学拉曼光谱以及同步辐射X射线吸收谱协同表征缺陷催化剂在真实电化学反应过程中缺陷演变以及调控本质。实现高活性、高选择性电催化剂的制备的同时系统解析缺陷调控本质以及活性制约因素。

Electrochemical reduction of CO2 is the ideal methods to solve CO2 emissions, but it still faces problems such as conversion efficiency and product selectivity. In recent years, the defects regulation of electrocatalyst has been widely studied and proved to be effective in improving its conversion efficiency and selectivity. However, the current defect preparation methods cannot achieve coordinated control of defect type, concentration and spatial distribution. At the same time, current research still lacks a systematic and in-depth understanding of the defect dynamic evolution and the defect regulation essence under real electrochemical working conditions. As an industrialized surface modification technology, ion beam irradiation has the merits of high precision and high controllability. It can produce different types and concentrations defects into the material to precisely modulate the electronic properties and catalytic activity. Therefore, this project will use ion beam irradiation to construct defects in transition metal oxides, and systematically study the relationship between CO2 reduction reaction activity and defect types, concentration, and distribution in materials. Furthermore, in-situ electrochemical Raman spectroscopy and synchrotron radiation X-ray absorption spectroscopy will be used to synergistically characterize the evolution of defects and the regulation essence of defect catalysts in the real electrochemical reaction process. Realize high-activity and high-selectivity electrocatalysts preparation while systematically analyzing the nature of defect regulation and activity constraints.