Oxygen functionalized diamond nanocone arrays coupling cobalt phthalocyanine for enhanced electrochemical CO2 reduction

Abstract

The development of high-efficiency catalysts plays a crucial role in advancing CO2 electroreduction techniques. Among potential candidates, diamond-based electrocatalysts show promise due to their broad electrochemical windows, which effectively suppress competitive hydrogen evolution and ensure high CO2 reduction efficiency. In this study, we report an integrated electrode composed of oxygen-terminated diamond nanocone (ODcone) with CoPc-molecules anchoring (CoPc/ODcone). The CoPc/ODcone electrodes exhibited remarkable performance, achieving a maximum Faradaic efficiency (FE) of 94.1% for CO at −0.97 V vs reversible hydrogen electrode (RHE), and maintaining an FECO higher than 80% over a wide potential range of −0.67 V to −1.07 V vs RHE. The outstanding performance of the CoPc/ODcone electrode can be attributed to the synergistic effects between the nanostructured diamond surface and the CoPc catalyst. The hydroxyl-rich nature of the diamond surface facilitates the anchoring of CoPc molecules and bonding with Co atoms in CoPc. Simultaneously, the nanostructured diamond with sharp tips enhances CO2 adsorption, thereby improving the catalyst's performance. This study provides valuable insights into the utilization of non-metallic carbon materials, particularly diamond, as metal-free catalysts in CO2 electrochemical reduction and tackles challenges such as low current density and poor Faradaic efficiency, thus contributing to the advancement of more effective catalysts for CO2 electroreduction.