Highly Durable Rh Single Atom Catalyst Modulated by Surface Defects on Fe‐Ce Oxide Solid Solution

/FC reduced at 300 °C. This Rh single-atom structure was sustained after 100 hours of CO-SCR at 400 °C. Reaction intermediates formed on the catalyst surface were analyzed using in situ diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS) under NO and CO flow conditions. Additionally, the catalyst structure and the CO-SCR reaction mechanism were investigated using density functional theory (DFT). While Rh atoms located near surface Fe sites were found to be thermodynamically most stable, both NO and CO preferentially adsorbed on Rh sites. Fe plays a role in stabilizing Rh sites and facilitating oxygen transfer. This work provides valuable insights into the design of highly active and durable single-atom catalysts.