Highly efficient electroconversion of carbon dioxide into hydrocarbons by cathodized copper-organic frameworks

Abstract

Highly selective conversion of carbon dioxide (CO2) into valuable hydrocarbons is promising yet challenging in developing effective electrocatalysts. Herein, CuII/adeninato/carboxylato metal-biomolecule frameworks (CuII/ade-MOFs) are employed for efficient CO2 electro-conversion towards hydrocarbon generation. The cathodized CuII/ade-MOF nanosheets demonstrate excellent catalytic performance for CO2 conversion into valuable hydrocarbons with a total hydrocarbon faradaic efficiency (FE) of over 73%. Ethylene (C2H4) is produced with a maximum FE of 45% and a current density of 8.5 mA cm-2 at -1.4 V vs. RHE, while methane (CH4) is produced with a FE of 50% and current density of ∼15 mA cm-2 at -1.6 V vs. RHE. These investigations reveal that the reconstruction of cathodized CuII/ade-MOFs and the formed Cu nanoparticles functionalized by nitrogen-containing ligands contribute to the excellent CO2 conversion performance. Furthermore, this work would provide valuable insights and opportunities for the rational design of Cu-based MOF catalysts for highly efficient conversion of CO2 towards hydrocarbon generation.