Operando Insights on the Direct Oxidation of Methane over Fe-SSZ-13

Based on prior knowledge regarding the interaction of N2O/O2 and CH4 with Fe in Fe-SSZ-13, this proposal aims to use an operando multi-spectroscopy approach including RIXS, KBeta-HERFD-XAS, and KBeta,alfa-XES to elucidate the temperature-dependent reaction mechanism of CH4 hydroxylation to CH3OH and to isolate the atomic-scale reactivity of active Fe centres. This includes monitoring the Fe oxidation state, the structure of intermediates (Fe-O), spin dynamics, and preferential ligation as a function of reaction conditions.

基于Fe-SSZ-13中N₂O/O₂与CH₄和Fe相互作用的已有知识，本研究计划旨在采用原位多光谱方法（包括共振非弹性X射线散射（RIXS）、β线高能量分辨荧光检测X射线吸收光谱（KBeta-HERFD-XAS）及β和α线X射线发射光谱（KBeta,alfa-XES）），阐明CH₄羟基化生成CH₃OH的温度依赖反应机制，并解析活性Fe中心在原子尺度的反应性。这包括监测Fe的氧化态、中间体（Fe-O）结构、自旋动力学及优先配位情况随反应条件的变化。