Theoretical investigation of CO2 conversion on corrugated g-C3N4 Surface decorated by single-atom of Fe, Co, and Pd

The conversion of CO2 molecules to useful fuels and value-added chemicals is important for protecting the atmosphere and developing a stable environment for humans. Therefore, the design of high-efficiency catalysts for CO2 adsorption, activation, and conversion has received considerable attention in recent decades. In this study, to investigate CO2 adsorption, activation, and dissociation on a decorated corrugated graphitic carbon nitride (gC3N4) surface, we conducted density-functional theory (DFT) calculations. Owing to the synergetic effect between the metal and g-C3N4, the decoration of the surface enhances the catalytic activity of CO2 activation. The catalyst structures, CO2 adsorption configurations, and electronic properties for CO2 activation on a decorated gC3N4 surface with dispersed transition metal single-atoms of Fe, Co, and Pd were investigated. The transition states for direct dissociation to form CO were obtained from the adsorbed CO2 to reveal the properties of activated carbon dioxide. Our calculations indicate that Fe@g-C3N4 and Co@g-C3N4 are good candidates for CO2 capture. Especially, the former exists a better catalytic activity for the CO2 activation. Additionally, DFT studies were combined with microkinetic simulations to comprehend the CO2 consumption and CO production reaction temperature on a single-atom decorated corrugated g-C3N4 surface.