Operando XAS analysis of visible light assisted CO2 reduction on mono- and bi-metallic (Ni, Cu,Fe)/ CeO2 catalysts

This proposal is aimed to analyze the active species in monometallic Ni or Cu, and bimetallic Ni-Cu subnanometer clusters dispersed on CeO2 or CeO2 doped with 8% Fe, during thermocatalytic and light-assisted CO2 reduction reactions. Operando X-ray absorption spectroscopy (XAS) coupled to MS will be used to simultaneously follow the oxidation state and local atomic structure of the (bi)metallic clusters and CeO2 support (with or without Fe dopant), as well as conversion and selectivity during thermally driven and light assisted CO2 reduction reactions. The obtained information will help to identify the dynamic interplay between the metals and the ceria support during the reaction and unravel the way visible light activates the metal@semiconductor photocatalyst.

本研究旨在分析分散于二氧化铈（CeO₂）或掺杂8%铁（Fe）的二氧化铈载体上的单金属镍（Ni）、铜（Cu）以及双金属镍-铜（Ni-Cu）亚纳米团簇，在热催化与光辅助二氧化碳还原反应中的活性物种。将采用与质谱（Mass Spectrometry, MS）联用的原位X射线吸收光谱（Operando X-ray absorption spectroscopy, XAS），同时追踪（单/双）金属团簇及（掺杂或未掺杂铁的）二氧化铈载体的氧化态与局部原子结构，同步监测热驱动及光辅助二氧化碳还原反应过程中的反应物转化率与产物选择性。所获信息将有助于阐明反应过程中金属与二氧化铈载体间的动态相互作用，揭示可见光激活金属@半导体光催化剂的内在机制。