Single Metal Atom catalysts electrochemical Reduction of CO2-To-CO (SMART-CO)

Achieving net zero CO2 emissions requires replacing fossil fuel-derived precursors in the chemical industry, driving the rise of the Power-to-X electrochemical sector. CO2 can be electrochemically reduced into valuable products at cost-competitive prices. Earth abundant single metal atoms coordinated to N-doped C (M-N-C, M = Fe, Ni) can selectively reduce CO2 to CO (an important precursor to Fischer-Tropsch and fermentation), with the same activity and efficiency as current commercially used thick Ag and Au electrode. M-N-C therefore present a cheaper, accessible, and sustainable alternative. However, their practical implementation is restricted by their synthesis bottlenecks, poorly understood CO2 reduction mechanism and long term (≥100 h) degradation at practical current densities (≥200 mA cm-2). To solve these problems, I will introduce automated M-N-C synthesis innovatively adapted from the food industry. State-of-the-art operando NMR will uniquely resolve the metal cation solvation and impact on CO2 reduction, while emerging electrochemical techniques and in-situ X-ray absorption spectroscopy will probe the active site density. I will calculate catalyst lifetimes for the first time, based on the rate of active site loss, and establish catalyst properties limiting stability. I will use these insights to develop an accelerated stress test for M-N-Cs in CO2 electrolysers, facilitating faster screening and establishing a benchmarking tool for academia and industry. Thus, the proposed project will solve the three major challenges of catalyst scalability, selectivity, and stability and would equip me with scientific, technical and managerial skills to become a leading independent researcher in electrochemical technologies. The world-leading M-N-C synthesis, reaction mechanism expertise and state-of-the-art equipment available with Dr. Fellinger (host); and the wide scientific community at BAM, provide a synergistic environment to successfully host my project.