Operando Vtc-XES and HERFD-XANES Studies on the Water Oxidation Mechanisms of Active Metal-Carbodiimides

Previously, we performed XAS studies to try to confirm the oxidation of Co centers and Co-O/-N/-C coordination. Due to the low resolution of those XAS experiments to distinguish O/N/C species with similar Z-number, we were not able to resolve the real active local-structure driving OER in CoNCN/CNTs. In this proposal, we aim to perform operando Vtc-XES and HERFD-XANES experiments to monitor the local-structure reconstruction processes in metal carbodiimides on carbon nanotubes (MNCN/CNT, M=Co/Fe/Ni) and unravel the effective coordination of metal centers for improved electrocatalysis. The Vtc-XES sensitivity to identify light C/N/O atoms in complex metallic matrixes, will allow us to determine the energy shifts in the ligand 2s ionization energies of bound C/N/O species upon catalytic activation. This will offer in-depth understandings on the structure-function relationships between coordinating O/N/C atoms and metal centers for designing high-performance MNCN-based electrocatalysts.