From Molecules to Modules: Pathways toward Scalable Electrochemical CO₂ Reduction.

Area of Science:

• Electrochemistry and catalysis for sustainable energy and chemical production.
• Materials science and engineering for advanced electrode design.
• Chemical engineering for process scale-up and industrial application.

Background:

• Achieving carbon neutrality necessitates robust carbon capture, utilization, and storage (CCUS) technologies.
• Electrochemical carbon dioxide reduction (CO2R) offers a pathway to convert CO2 and water into fuels using renewable electricity.
• Current lab-scale CO2R technologies face challenges in scalability, catalyst development, transport phenomena understanding, and electrolyzer design.

Purpose of the Study:

• To describe chemistry and engineering methodologies for advancing large-scale CO2R.
• To bridge the knowledge gap between molecular-level understanding and process engineering for CO2R scale-up.
• To provide a roadmap for developing techno-economically viable CO2R technologies.

Main Methods:

• Utilized descriptor-based neural networks for rational screening and design of high-performance electrocatalysts (alloys and single-atom sites).
• Employed advanced coating and fabrication techniques for durable catalyst layers in gas diffusion electrodes (GDEs).
• Developed device design requirements for CO2 electrolysis under elevated pressure and temperature to address scale-up challenges.

Main Results:

• Demonstrated tailored reactivity of rationally designed catalysts through neural network screening.
• Improved electrode performance by managing interfacial resistances and controlling gas-liquid equilibria in GDEs.
• Proposed design principles for electrolyzers capable of efficient, large-scale CO2 conversion.

Conclusions:

• Integrating fundamental molecular insights with rigorous process design is critical for industrial CO2R.
• Advanced catalyst design and electrode fabrication are essential for efficient and durable CO2R systems.
• Addressing transport phenomena and electrolyzer design is key to scaling up CO2R technology for carbon neutrality goals.