Bridging Thermal Catalysis and Electrocatalysis: Catalyzing CO₂ Conversion with Carbon-Based Materials

Area of Science:

• Materials Science and Catalysis
• Electrochemistry and Thermocatalysis

Background:

• Distinguishing between temperature- and electric potential-driven reactions is difficult due to material limitations in thermal and electrocatalytic settings.
• Developing unified catalytic systems requires understanding shared mechanisms across different reaction environments.

Purpose of the Study:

• To investigate the catalytic behavior of Ni, N-doped carbon (NiPACN) in both thermal and electrochemical CO2 conversion.
• To establish an analogy between thermal (reverse water-gas shift) and electrochemical (CO2 reduction) catalysis using a single material.

Main Methods:

• Utilized Ni, N-doped carbon (NiPACN) as a catalyst for both thermal and electrochemical CO2 conversion.
• Employed advanced characterization techniques to analyze the catalyst's active sites and reaction mechanisms.
• Developed a generalized reaction driving-force model incorporating temperature and electrical potential.

Main Results:

• NiPACN selectively catalyzes thermal CO2 to CO via the reverse water-gas shift (RWGS) reaction, analogous to its electrochemical CO2 reduction (CO2 R) activity.
• Advanced characterization indicates that dispersed Ni sites on NiPACN are responsible for facilitating the RWGS reaction.
• The study suggests NiPACN may exhibit faster kinetics for CO2 R compared to RWGS due to lower intrinsic energy barriers.

Conclusions:

• NiPACN serves as a versatile catalyst, enabling direct comparison between thermal and electrochemical reaction pathways.
• The findings highlight the potential for a unified understanding of catalytic phenomena across disparate reaction environments.
• This work encourages further research into quantitatively linking catalytic behaviors in varied conditions.