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.