Boosting CO2 Reduction on Fe-N-C with Sulfur Incorporation: Synergistic Electronic and Structural Engineering

This study reports a general strategy to boost electrocatalytic CO2RR activity of Fe-N-C with the incorporation of S atoms to engineer carbon support structure and electronic properties of active Fe−N sites simultaneously via a copolymer-assisted synthetic approach. The employment of N,S comonomers significantly increases the numbers of micropores and surface area, enabling dense atomic Fe−N and enhanced utilization efficiency. The first-principles calculations reveal that S modulation upraises the Fermi energy of Fe 3d and increases charge density on Fe atoms of Fe−N4, thereby enhancing intrinsic catalytic reactivity and selectivity for CO2 reduction by strengthening the binding interaction between the Fe site and key COOH* intermediate. These integrated structural and electronic merits endow Fe-NS-C with outstanding activity (e.g., CO Faradaic efficiency of 98% at an overpotential of 490 mV) and stability (without deactivation in 30 h), ranking it one of the most active Fe-N-C reported to date. The finding offers an innovative design strategy to enable the design of advanced catalysts for CO2 conversion.Graphical abstractSulfur addition promotes electrocatalytic CO2 reduction on Fe-N-C by synergistically tailoring structure of carbon support and electronic properties of single atomic Fe−N sites, achieving top-level performance for CO generation among Fe-N-C catalysts.
Source: Nano Energy - Category: Nanotechnology Source Type: research