Bridging Thermal Catalysis and Electrocatalysis: Catalyzing CO 2 Conversion with Carbon‐Based Materials

• Published in: Angewandte Chemie International Edition Vol. 60; no. 32; pp. 17472 - 17480
• Main Authors: Koshy, David M., Nathan, Sindhu S., Asundi, Arun S., Abdellah, Ahmed M., Dull, Samuel M., Cullen, David A., Higgins, Drew, Bao, Zhenan, Bent, Stacey F., Jaramillo, Thomas F.
• Format: Journal Article
• Language: English
• Published: 02.08.2021
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202101326

Abstract Understanding the differences between reactions driven by elevated temperature or electric potential remains challenging, largely due to materials incompatibilities between thermal catalytic and electrocatalytic environments. We show that Ni, N‐doped carbon (NiPACN), an electrocatalyst for the reduction of CO 2 to CO (CO 2 R), can also selectively catalyze thermal CO 2 to CO via the reverse water gas shift (RWGS) representing a direct analogy between catalytic phenomena across the two reaction environments. Advanced characterization techniques reveal that NiPACN likely facilitates RWGS on dispersed Ni sites in agreement with CO 2 R active site studies. Finally, we construct a generalized reaction driving‐force that includes temperature and potential and suggest that NiPACN could facilitate faster kinetics in CO 2 R relative to RWGS due to lower intrinsic barriers. This report motivates further studies that quantitatively link catalytic phenomena across disparate reaction environments.