SAC-Cu-CO2RR · Highly Ethanol-Selective Electrocatalytic CO2 Reduction Enabled by Site-Specific Heteroatoms Doped Single Atom Catalysts Supported Cu Clusters

Electrochemical CO2 reduction reaction (CO2 RR) driven by renewable power is a promising way to convert CO2 to fuels and chemicals, which has been proposed as a sustainable process for the artificial carbon cycle. Among all products, ethanol (C2H5OH) has received extensive attention because it can be directly used as fuel in internal combustion engines and industrial power generation. Cu-based catalysts can efficiently promote C-C coupling toward C2+ products in CO2 RR. However, most Cu-based catalysts still show an insufficient selectivity for C2H5OH (<50 %) due to unfavorable adsorption of several oxygen-containing key intermediates, which cannot achieve its commercial value. As a frontier in materials science, single-atom motifs anchored on N-doped C support (carbon-based SACs), are widely investigated due to their maximum atom-utilization efficiency and highly metal dispersion. Especially, in the field of eCO2 RR, compared to the pure N-C, SACs exhibit an excellent CO selectivity because of the easily optimized coordination environment along with a reconstructed structure. Therefore, combining SACs with Cu-based catalysts in the proper configuration can increase the local CO concentration near Cu-based materials at a low overpotential where Cu alone would be incapable of doing the CO2-to-CO conversion. Meanwhile, the moderate electron-donating ability of SACs will further stabilize the oxygenic C2 intermediate to make the hydrogenation pathway toward C2H5OH production more favorable. As a result, the objective of this project is to design a carbon-based SACs supported Cu clusters architecture by a chemical in-situ growth process to let it serve as a high-efficient catalyst for achieving a high C2H5OH selectivity (> 75 %) at a low overpotential (< 800 mV). This project will set the scene for the fabrication of highly efficient and commercially available electrodes for the eCO2 RR to production of C2H5OH.