Conversion of CO2 into useful fuels by electrochemical CO2 reduction (CO2RR) requires earth-abundant catalysts with efficient performance. Limited achievement on either catalytic performance or reaction mechanism in iron and nitrogen co-doped carbon (Fe-N-C) restricts the development of CO2RR on those catalyst systems. In our work, a copolymer-assisted synthetic approach was used to enhance electrocatalytic performance of Fe-N-C by incorporating sulfur into the carbon lattice. Surface structure and electronic properties were significantly improved by the S addition. Higher surface area and porosity enabled more uniform Fe dispersion into atomic Fe-N states, providing one of the most outstanding performance reported in the literature. 98% CO selectivity at an overpotential of 490 mV and the long stability without deactivation in 30 h were achieved in this work. In addition, first principle calculations were carried out to analyze the significance of S addition. The results revealed that the Fermi energy of Fe 3d was upraised and the charge density on Fe was increased by S, giving more active property to the Fe-N sites to interact with the key intermediate COOH* in the whole CO2 reduction pathways.

Engineering Iron/Nitrogen/Sulfur co-doped carbon catalysts for efficient electrochemical CO2 reduction

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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