Well-defined copper nanocrystals to control selectivity in CO2 and CO electroconversion

Anna Loiudice^a, Min Wang^a, Enric Ibáñez Alé^b, Krishna Kumar^a, Dragos Stoian^c, Zan Lian^b, Petru Albertini^a, Ludovic Zaza^a, Jari Leeman^a, Nuria Lopez^b, Raffaella Buonsanti^a

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

^bInstitute of Chemical Research of Catalonia (ICIQ-CERCA), The Barcelona Institute of Science and Technology (BIST), Av. Països Catalans, 16, 43007 Tarragona, Spain.

^cSwiss-Norwegian Beamlines, European Synchrotron Radiation Facility (ESRF), Grenoble, France.

Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)

#PECCO2 - Advances in (Photo)Electrochemical CO2 Conversion to Chemicals and Fuels

Lausanne, Switzerland, 2024 November 12th - 15th

Organizers: Deepak PANT, Adriano Sacco and juqin zeng

Oral, Anna Loiudice, presentation 155
Publication date: 28th August 2024

Correlating activity, selectivity and stability with the structure and composition of catalysts is crucial to advance the knowledge in chemical transformations which are essential to move towards a more sustainable economy. Among these, the electrochemical CO2 reduction reaction(CO2RR) and, more recently, CO reduction reaction (CORR) hold the promise to close the carbon cycle by storing renewable energies into chemical feedstocks. Although notable progress has been made in understanding the parameters which govern activity and selectivity in CO2RR, CORR is still in its infancy. Catalyst stability remains a less explored property for both reactions.

In this talk, I will show how well-defined copper nanocrystals (NCs) synthesized via colloidal synthesis can be used as model system to establish unambiguous structure/property relations in CO2RR and CORR.

First of all, I will illustrate how tailor made copper NCs have revealed synergy between shape and size, thus the importance of facet ratio in CO2RR.[1] Secondly, I will show that these relationships hold when these catalysts are integrated in a gas-fed electrolyzers at technologically relevant conditions with currents up to 300 mA/cm2.[2]

I will then present our recent advancement in understanding structural dependence relationship in CORR. Specifically, I will discuss about the importance of lattice strain for the production of alcohols in this reaction as revealed by a combination of theoretical simulation and advanced characterization techniques. I will close with a discussion of stability of these catalysts and compare CO2RR/CORR conditions. [3]

References:

[1] A. Loiudice, P. Lobaccaro, E. A. Kamali, T. Thao, B. H. Huang, J. W. Ager, R. Buonsanti “Tailoring Copper Nanocrystals towards C2 Products in Electrochemical CO2 Reduction” Angew.Che m. Int. Ed. 2016, 55, 5789–5792.

[2] G. L. De Gregorio, T. Burdyny, A. Loiudice, P. Iyengar, W. A. Smith, R. Buonsanti “Facet-Dependent Selectivity of Cu Catalysts in Electrochemical CO2 Reduction at Commercially Viable Current Densities” ACS Catal. 2020, 10, 9, 4854–4862.

[3] J. Vavra, G. P. L. Ramona, F. Dattila, A. Kormányos, T. Priamushko, P. P. Albertini, A. Loiudice, S. Cherevko, N. Lopéz, R. Buonsanti “Solution-based Cu+ transient species mediate the reconstruction of copper electrocatalysts for CO2 reduction” Nature Catal. 2024, 7, 89.

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