Perfluorinated Covalent Triazine Framework Derived Hybrids for the Highly Selective Electroconversion of Carbon Dioxide into Methane

Developing cost-effective electrocatalysts for high-selectivity CO2 electroreduction remains challenging. We herein report a perfluorinated covalent triazine framework (CTF) electrocatalyst that displays very high selectivity in the electroreduction of CO2 to CH4 with a faradaic efficiency of 99.3% in aqueous electrolyte. Systematic characterization and electrochemical studies, in combination with density functional theory calculations, demonstrate that the presence of both nitrogen and fluorine in the CTF provides a unique pathway that is inaccessible with the individual components for CO2 electroreduction.