Regulating the electrocatalytic active centers for accelerated proton transfer towards efficient CO₂ reduction

Area of Science:

• Electrochemistry
• Catalysis
• Materials Science

Background:

• Electrochemical CO2 reduction (CO2RR) is crucial for energy and environmental solutions.
• Slow proton-coupled electron transfer hinders CO2RR catalytic performance.
• Optimizing the catalyst's local structure can enhance reaction kinetics.

Purpose of the Study:

• To develop a novel catalyst for efficient CO2 and H2O co-reduction.
• To investigate the role of catalyst structure in enhancing CO2RR kinetics.
• To understand the mechanism of microenvironment optimization in CO2RR.

Main Methods:

• Synthesis of cubic-phase α-MoC1-x nanoparticles integrated into a carbon matrix and coupled with cobalt phthalocyanine (α-MoC1-x-CoPc@C).
• Electrochemical measurements and in-situ spectroscopies.
• Theoretical simulations to analyze catalyst structure and reaction mechanisms.

Main Results:

• The α-MoC1-x-CoPc@C catalyst achieved near 100% Faradaic efficiency for CO production.
• α-MoC1-x and CoPc acted as active sites for H2O activation and CO2 reduction, respectively.
• An optimized interfacial water network enhanced water dissociation and proton transfer.

Conclusions:

• The engineered microenvironment at the electrode-electrolyte interface significantly improves CO2RR performance.
• The catalyst design provides a novel strategy for enhancing catalytic efficiency in CO2 reduction.
• This work offers insights into synergistic effects between catalyst structure and reaction environment.