Novel Copper-Nickel Pc-Por-Based Electrocatalysts for Highly Selective CO2 Reduction and Multi-Carbon Compound Synthesis

Efforts are focused on developing an efficient strategy to combat global warming while also advancing the electrochemical conversion of carbon dioxide (CO2) into multi-carbon compounds and improving C-C coupling processes. For accelerating the transformation of CO2 into high-value chemicals, Metallomacrocyclic compounds have shown great potential among the many materials under investigation. However, they have thus far run across issues including low current density, limited catalytic activity, poor product selectivity, and stability worries. In this work, we present a novel achievement in the form of stable and conductive ultrathin dimeric Copper-Nickel Pc-Por-based electrocatalysts, synthesized through a solvent-assisted strategy. The manipulation of electron polarization between metal atoms is made feasible by adjusting the functionality and size of ligands, which enhances catalytic activity. This, in turn, leads to heightened atom utilization efficiency, customized catalytic behaviors, and exceptional selectivity, surpassing the benchmarks in C-C coupling and multi-carbon product formation. Our electrocatalyst exhibits remarkable selectivity for acetylene production, as demonstrated in an H-type cell. When operating in a 0.5 M KHCO3 solution, it achieves outstanding Faradaic efficiencies (FEs) for CO2 reduction at 0.61 V (vs. RHE), yielding over 94% acetylene with a current density exceeding 85 mA cm2. These results surpass the performance of the majority of previously reported CO2 electrocatalysts. This study introduces a practical approach for designing future generations of cost-effective, efficient, and selectivity electrocatalytic reduction of carbon dioxide, offering potential solutions to mitigate global warming.