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

Abstract Developing cost‐effective electrocatalysts for high‐selectivity CO 2 electroreduction remains challenging. We herein report a perfluorinated covalent triazine framework (CTF) electrocatalyst that displays very high selectivity in the electroreduction of CO 2 to CH 4 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 CO 2 electroreduction.