A Versatile Synthetic Method for Screening Bimetallic Catalysts for CO2 Electroreduction

Laura C. Pardo Perez^a, Zora Chalkley^a, Alvaro Diaz Duque^a, Matthew T. Mayer^a

^aHelmholtz-Zentrum Berlin für Materialien und Energie GmbH, Hahn-Meitner-Platz 1, 14109 Berlin, Germany.

Proceedings of International Conference on Frontiers in Electrocatalytic Transformations (INTERECT)

València, Spain, 2021 November 22nd - 23rd

Organizers: Elena Mas Marzá and Ward van der Stam

Contributed talk, Laura C. Pardo Perez, presentation 021
DOI: https://doi.org/10.29363/nanoge.interect.2021.021
Publication date: 10th November 2021

The electrochemical reduction of carbon dioxide (CO₂ER) offers a sustainable approach for CO₂ reutilization and conversion into added value chemicals. A wide variety of products can be formed during CO₂ER such as formate, CO, hydrocarbons and alcohols and therefore tuning the selectivity of CO₂ER catalysts remains a major challenge in the field.

The initial reduction of CO₂ (2e-) can yield formate or CO. While the former is commonly accepted as a terminal product which can’t be further reduced, CO has been demonstrated to be a key intermediate in the formation of higher reduction products ( >2e-) such as hydrocarbons and alcohols.^[1] The CO₂ and CO binding strength on the metal surface are key factors determining the selectivity.^[2] Post transition metals like Sn, In, Ga have weak interaction with CO₂ and are known to favor formate production.^[3–5] Au and Ag that adsorb CO weakly release it as final product. Pt, Ni, Fe and Co that bind CO too strongly are poisoned and unable to further reduce it, suppressing CO₂R and favoring HER. Cu stands out as the only metallic surface characterized by an intermediate CO binding strength that favors further reduction to hydrocarbons or alcohols. Bimetallic catalysts offer possible synergetic effects among different metals to yield optimal binding of CO as key intermediate and have been demonstrated as an approach for tuning selectivity in Cu based catalysts ^[6,7]

Here we present the screening of bimetallic composites as CO₂ER electrocatalysts using a facile synthesis by spin coating of metal precursors in solution to form mixed oxides (M_AM_BOx) thin films. We focus on combining early transition metals traditionally known to bind CO strongly and favor HER (M_A=Fe, Ni or Co) with post-transition metals (M_B= In, Sn or Ga), known to suppress HER. The influence of metal composition on CO₂ER selectivity will be discussed, along with the structural changes observed in the composites during in situ reduction

References:

[1] Hori, Y.; Murata, A.; Takahashi, R. Formation of Hydrocarbons in the Electrochemical Reduction of Carbon Dioxide at a Copper Electrode in Aqueous Solution. J. Chem. Soc. Faraday Trans. 1 Phys. Chem. Condens. Phases 1989, 85 (8), 2309.

[2] Peterson, A. A.; Nørskov, J. K.; Norskov, J. K. Activity Descriptors for CO 2 Electroreduction to Methane on Transition-Metal Catalysts. J. Phys. Chem. Lett. 2012, 3 (2), 251–258.

[3] Azuma, M. Electrochemical Reduction of Carbon Dioxide on Various Metal Electrodes in Low-Temperature Aqueous KHCO3 Media. J. Electrochem. Soc. 1990, 137 (6), 1772.

[4] Ikeda, S.; Takagi, T.; Ito, K. Selective Formation of Formic Acid, Oxalic Acid, and Carbon Monoxide by Electrochemical Reduction of Carbon Dioxide. Bulletin of the Chemical Society of Japan. 1987, pp 2517–2522.

[5] Mahmood, M. N.; MAsheder, D.; Harty, C. J. Use of Gas-Diffusion Electrodes for High Rate Electrochemical Reduction of Carbon Dioxide.I. Reduction at Lead , Indium and Tin Impregnated Electrodes. J. Appl. Electrochem. 1987, 17, 1159–1170.

[6] Vasileff, A.; Xu, C.; Jiao, Y.; Zheng, Y.; Qiao, S. Z. Surface and Interface Engineering in Copper-Based Bimetallic Materials for Selective CO2Electroreduction. Chem 2018, 1–23.

[7] Birhanu, M. K.; Tsai, M.-C.; Kahsay, A. W.; Chen, C.-T.; Zeleke, T. S.; Ibrahim, K. B.; Huang, C.-J.; Su, W.-N.; Hwang, B.-J. Copper and Copper-Based Bimetallic Catalysts for Carbon Dioxide Electroreduction. Adv. Mater. Interfaces 2018, 5 (24), 1800919.

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