Solid-liquid electrocatalysts for the CO2 reduction

Coline Boulanger^a, Haoxuan You^a, Krishna Kumar^a, Petru P. Albertini^a, Jari Leemans^a, Valery Okatenko^a, Raffaella Buonsanti^a

^aLaboratory of Nanochemistry for Energy Research, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne, Sion, CH-1950, Switzerland

Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)

#PhotoDeg - Materials and devices for stable and efficient solar fuels

Lausanne, Switzerland, 2024 November 12th - 15th

Organizers: Sophia Haussener, Sandra Luber and Simone Pokrant

Oral, Coline Boulanger, presentation 057
Publication date: 28th August 2024

One of the current issues in the electrochemical CO2 reduction reaction (CO2RR) is the stability of the catalyst. [1] Copper is the most promising material for producing desirable C2+ chemicals at reasonable rate, yet this metal reconstructs during operation. [1] A solution is to either block this reconstruction or to learn how to direct it towards structures with the desired selectivity. [2]

Herein, we propose to explore a different class of materials. These materials are liquid metal Ga-based nanoparticles (NPs). We propose them as alternative to traditional solid catalysts with great potential for stable CO2RR thanks to their self-regenerating dynamic surface. [3,4] Yet, we are still learning about their chemistry, which is at its infancy compared to other NPs. [5,6] Developing their chemistry is important to further explore them for selectivity in CO2RR and eventually for other reactions.

In this talk, we will focus on the most recent work where we synthetize tunable and monodisperse Ga-based NPs incorporating a variety of different metals through colloidal chemistry. In particular, we prepare solid-liquid-solid Ga-M NPs (M= Ag, Cu, Au, Pd) wherein a solid metal is encapsulated within a liquid Ga NP confined by its oxide skin. We elucidate the formation mechanism of these unique nanostructures through a combination of state-of-the-art in-situ techniques, including electron microscopy and X-ray absorption spectroscopy. Finally, we demonstrate the functionality of these NPs as CO2RR electrocatalysts.

References:

[1] Popović, S.; Smiljanić, M.; Jovanovic, P.; Vavra, J.; Buonsanti, R.; Hodnik, N. Stability and Degradation Mechanisms of Copper-Based Catalysts for Electrochemical CO2 Reduction. Angew. Chem., Int. Ed., 2020, 59, 14736–14746

[2] Albertini, P.; Newton, M. A.; Wang, M.; Segura Lecina, O.; Green, P. B.; Stoian, D. C.; Oveisi, E.; Loiudice, A.; Buonsanti, R. Nature Materials, 2024, 23, 680-687

[3] Okatenko, V.; Castilla-Amorós, L.; Stoian, D. C.; Vávra, J.; Loiudice, A.; Buonsanti, R. The Native Oxide Skin of Liquid Metal Ga Nanoparticles Prevents Their Rapid Coalescence during Electrocatalysis. J. Am. Chem. Soc. 2022, 144, 10053–10063

[4] Okatenko, V.; Loiudice, A.; Newton, M. A.; Stoian, D. C.; Blokhina, A.; Chen A. N.; Rossi, K.; Buonsanti, R. Alloying as a Strategy to Boost the Stability of Copper Nanocatalysts during the Electrochemical CO2 Reduction Reaction. J. Am. Chem. Soc. 2023, 125, 9, 5370-5383

[5] Castilla-Amorós, L.; Stoian, D. C.; Pankhurst, J. R.; Varandili, S. B.; Buonsanti, R. Exploring the Chemical Reactivity of Gallium Liquid Metal Nanoparticles in Galvanic Replacement. J. Am. Chem. Soc. 2020, 142, 45, 19283-19290

[6] Okatenko, V.; Boulanger, C.; Chen, A. N. ; Kumar, K. ; Schouwink, P.; Loiudice, A.; Buonsanti, R. Voltage-Driven Chemical Reactions Enable the Synthesis of Tunable Liquid Ga–Metal Nanoparticles. J. Am. Chem. Soc. 2023, 145, 46, 25401-25410

Acknowledgements:

This work was supported by the Swiss State Secretariat for Education, Research and Innovation (SERI) under contract number MB22.00065.

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