Implanting Numerous Hydrogen-Bonding Networks in a Cu-Porphyrin-Based Nanosheet to Boost CH4 Selectivity in Neutral-Media CO2 Electroreduction

The exploration of novel systems for the electrochemical CO2 reduction reaction (CO2RR) for the production of hydrocarbons like CH4 remains a giant challenge. Well-designed electrocatalysts with advantages like proton generation/transferring and intermediate-fixating for efficient CO2RR are much preferred yet largely unexplored. In this work, a kind of Cu-porphyrin-based large-scale (approximate to 1.5 mu m) and ultrathin nanosheet (approximate to 5 nm) has been successfully applied in electrochemical CO2RR. It exhibits a superior FECH4 of 70 % with a high current density (-183.0 mA cm(-2)) at -1.6 V under rarely reported neutral conditions and maintains FECH4 >51 % over a wide potential range (-1.5 to -1.7 V) in a flow cell. The high performance can be attributed to the construction of numerous hydrogen-bonding networks through the integration of diaminotriazine with Cu-porphyrin, which is beneficial for proton migration and intermediate stabilization, as supported by DFT calculations. This work paves a new way in exploring hydrogen-bonding-based materials as efficient CO2RR catalysts.

Automated summary

This study successfully utilized a Cu-porphyrin-based large-scale and ultrathin nanosheet as an electrocatalyst for CO2RR, achieving high CO2 conversion efficiency under neutral conditions. By constructing hydrogen-bonding networks, proton migration and intermediate stabilization were facilitated, providing a new pathway for efficient CO2RR catalyst development.