Heterogeneous Electrochemical Carbon Dioxide Reduction in Aqueous Medium Using a Novel N4-Macrocyclic Cobalt Complex

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Molecular catalysts offer tunable electronic structures for electrochemical carbon dioxide reduction (CO2RR).
• Developing efficient and stable catalysts for CO2RR in aqueous environments is crucial for sustainable technologies.

Purpose of the Study:

• To synthesize and characterize a novel N4-macrocyclic cobalt complex for heterogeneous electrochemical CO2RR.
• To evaluate the catalytic performance of the cobalt complex in aqueous media.
• To investigate the role of the quaterpyridine moiety in CO2 conversion.

Main Methods:

• Synthesis of an N4-macrocyclic cobalt complex via dimerization coupling.
• Electrochemical CO2RR experiments in an aqueous environment.
• Online mass spectrometry and in situ attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR) for product analysis.
• Computational modeling to elucidate the catalytic mechanism.

Main Results:

• The synthesized cobalt complex effectively catalyzes CO2RR at low overpotentials.
• Near-unity carbon monoxide (CO) production was achieved over a wide potential range.
• The quaterpyridine moiety was identified as crucial for efficient CO2 conversion.
• Experimental data were corroborated by computational studies.

Conclusions:

• The novel cobalt complex with a quaterpyridine moiety demonstrates superior performance for electrochemical CO2RR in aqueous solutions.
• This study highlights the potential of such cobalt complexes for sustainable CO2 conversion.
• The findings contribute to the advancement of molecular electrocatalysis for CO2 utilization.