原位同步辐射研究铜基超薄材料电化学二氧化碳还原反应机制

电催化还原技术，可以在比较温和的条件下，将CO2转化为高价值的碳氢燃料，被认为是解决当前能源问题和温室效应的有效途径。Cu基纳米材料作为优异的CO2还原催化剂，受到了广泛的研究兴趣和关注。然而，对于Cu基纳米材料在CO2还原过程中的表面分子吸附活化、中间产物分子吸脱附转换、活性中心重构等催化本质缺乏清晰认知。本项目拟开发形貌及配位环境可控的Cu基超薄纳米材料，基于合肥光源光电子能谱线站发展同步辐射软X射线吸收谱（sXAS）与同步辐射光电子能谱（SRPES）联用技术，结合电化学原位反应装置，针对Cu基超薄纳米材料CO2电催化还原反应，实时在线观察表面反应物分子的吸脱附状态，中间产物的吸脱附及转变过程，以及Cu基催化剂表面原子价态、活性中心的原子和电子结构演化规律，从原子和分子尺度阐明催化反应机理及活性位结构，获得CO2电催化还原机制。并以此为指导，设计合成高效Cu基电催化CO2还原催化剂。

CO2 electrocatalytic reduction technology, which can convert CO2 into value-added hydrocarbon fuels under mild conditions, has been considered as an effecient way to solve the current energy crisis and greenhouse effect. As excellent catalysts for CO2 reduction reaction (CO2RR), Cu-based nanomaterials have attracted extensive interest and attention. However, the fundamental understanding of the intrinsic catalytic pathways, such as the adsorption and activation of reactants, conversion of the intermediates, and the reconstruction of active centers, during CO2RR remains unclear. Based on the soft X-ray absorption spectroscopy (sXAS), the synchrotron radiation photoelectron spectroscopy (SRPES) and in-situ reaction equipment at photoemission end-station in the National Synchrotron Radiation Laboratory (NSRL) in Hefei, this project aims to decipher the catalytic principle and acquire the key rate determining factor of copper-based ultrathin nanocatalysts for CO2RR in atomic levels, by in-situ investigating the adsorption and activation of reactants and probing the evolution of valence state and coordination environment of metal elements in nanocatalysts during CO2RR. This study could provide fundamental guidance for the rational design and synthesis of highly efficient Cu-based nanocatalysts for CO2RR.