Colloidal Multimetallic Nanoparticles to Advance Electrochemical CO2 Conversion Studies

Laia Castilla-Amorós^a, Jianfeng Huang^a, Raffaella Buonsanti^a

^aEcole Polytechnique Federale de Lausanne (EPFL), Lausanne, Switzerland

Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting19 (NFM19)

#SolCat19. (Photo)electrocatalysis for sustainable carbon utilization: mechanisms, methods, and reactor development

Berlin, Germany, 2019 November 3rd - 8th

Organizer: Matthew Mayer

Poster, Laia Castilla-Amorós, 380
Publication date: 18th July 2019

Because of the existence of linear scaling relationship, CO2RR requires more than one catalytic centre to proceed in an efficient manner.¹For this reason, the combination of multiple metallic elements via alloying or di/trimerization into an individual particle holds the promise to possess catalytic properties which exceeds those of single-element nanoparticles.

Multimetallic nanoparticles (MMNPS) are attracting increasing interest as catalysts for a wide range of reactions.^2,3Examples in CO2RR also show the advantage of combining copper, which is the only metal capable of catalysing the C-C bond formation, with other metals to improve selectivity (CuSn, CuZn, CuPd).^4–6Our group has recently demonstrated that Ag-Cu nanodimers, wherein two domain of Cu and Ag share an interface, promote C-C coupling due to synergistic tandem and electronic effects.⁷ Nevertheless, selectivity still needs improvement and other combinations of metals are required to optimize the binding energy of the intermediate. A recent theoretical study based on machine learning has identified CuGa as a promising candidate to achieve a near optimal binding energy of the CO intermediate.⁸

In this work, CuGa nanodimers were successfully synthesised by means of colloidal chemistry exploiting a galvanic replacement reaction. Ga nanoparticles were used as seeds to react with a Cu precursor. A combination of electron microscopy techniques was used to elucidate the reaction mechanism and to characterize the obtained dimers. UV-Vis absorption experiments suggest a charge transfer between Cu and Ga that could positively affect their functioning as catalysts for electrochemical CO2reduction. The generality of the developed synthetic approach was proven by synthesizing AuGa nanodimers and AgCuGa nanotrimers in which Ag and Cu were chemioselectively attached to Ga. These results established the viability of colloidally synthesised Ga NPs as initial precursors of a total synthesis scheme for colloidal non-noble metal based MMNPs.

References:

[1] Hansen, H. A., Varley, J. B., Peterson, A. A. & Nørskov, J. K. Understanding trends in the electrocatalytic activity of metals and enzymes for CO2 reduction to CO. J. Phys. Chem. Lett. 4, 388–392 (2013).

[2] Xie, P. et al. Highly efficient decomposition of ammonia using high-entropy alloy catalysts. Nat. Commun. 10, 1–12 (2019).

[3] Batchelor, T. A. A. et al. High-Entropy Alloys as a Discovery Platform for Electrocatalysis. Joule 3, 834–845 (2019).

[4] Sarfraz, S., T. Garcia-Esparza, A., Jedidi, A., Cavallo, L. & Takanabe, K. Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO2 to CO. ACS Catal. 6, 2842–2851 (2016).

[5] Feng, Y. et al. Laser-Prepared CuZn Alloy Catalyst for Selective Electrochemical Reduction of CO 2 to Ethylene. Langmuir 34, 13544–13549 (2018).

[6] Zhang, S. et al. Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane. Proc. Natl. Acad. Sci. U. S. A. 112, 15809–15814 (2015).

[7] Huang, J., Mensi, M., Oveisi, E., Mantella, V. & Buonsanti, R. Structural Sensitivities in Bimetallic Catalysts for Electrochemical CO2 Reduction Revealed by Ag-Cu Nanodimers. J. Am. Chem. Soc. 141, 2490–2499 (2019).

[8] Tran, K. & Ulissi, Z. W. Active learning across intermetallics to guide discovery of electrocatalysts for CO2 reduction and H2 evolution. Nat. Catal. 1, 696–703 (2018).

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