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

David M Koshy; Sindhu S Nathan; Arun S Asundi; Ahmed M Abdellah; Samuel M Dull; David A Cullen; Drew Higgins; Zhenan Bao; Stacey F Bent; Thomas F Jaramillo

doi:10.1002/anie.202101326

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

Angew Chem Int Ed Engl. 2021 Aug 2;60(32):17472-17480. doi: 10.1002/anie.202101326. Epub 2021 Jun 30.

Authors

David M Koshy^{1

2}, Sindhu S Nathan^{1

2}, Arun S Asundi^{1

2}, Ahmed M Abdellah³, Samuel M Dull¹, David A Cullen⁴, Drew Higgins³, Zhenan Bao^{1

2}, Stacey F Bent^{1

2}, Thomas F Jaramillo^{1

2}

Affiliations

¹ Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA, 94305, USA.
² SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd., Menlo Park, CA, 94025, USA.
³ Department of Chemical Engineering, McMaster University, 1280 Main St W, Hamilton, ON, L8S 4L8, Canada.
⁴ Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, 1 Bethel Valley Rd, Oak Ridge, TN, 37830, USA.

PMID: 33823079
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 CO₂ to CO (CO₂ R), can also selectively catalyze thermal CO₂ 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 CO₂ 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 CO₂ R relative to RWGS due to lower intrinsic barriers. This report motivates further studies that quantitatively link catalytic phenomena across disparate reaction environments.

Keywords: carbon dioxide; catalysis; electrochemistry; nitrogen-doped carbon; reverse water-gas shift.

Abstract

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