Copper-based hybrid nanomaterials for the electrocatalytic reduction of CO2

Joan Marc Bondia Pedra^a^,^b, Federico Franco^a, Carlos Puerto^a, Emilio Palomares-Gil^a^,^c

^aInstitute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, Tarragona 43007, Spain

^bDepartament d’Enginyeria Electrònica, Elèctrica i Automàtica, Universitat Rovira i Virgili, Avinguda dels Països Catalans, 26, Tarragona, Spain

^cICREA, Passeig LLuis Companys 23, E-08010, Spain

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)

#e-FuelSyn - Electrocatalysis for the Production of Fuels and Chemicals

VALÈNCIA, Spain, 2023 March 6th - 10th

Organizers: Carla Casadevall Serrano and Julio Lloret Fillol

Poster, Joan Marc Bondia Pedra, 334
Publication date: 22nd December 2022

Global warming, worldwide energy crisis and the issues related to increasing levels of carbon dioxide (CO₂) have prompted the research of new catalysts to transform CO₂ back to fuels and value-added chemicals [1]. Copper (Cu)-based nanocatalysts have attracted increasing interest in CO₂reduction over the last decades, due to their unique capability to promote an electrochemical reduction of CO₂into multicarbon C₂₊ products. Nevertheless, an efficient Cu-catalyst is required to face the typical high overpotentials required for the process and the low selectivity, which results in obtaining a mixture of several products (C₁-C₃) [2].

Combining molecular with heterogeneous chemistry has revealed to be an efficient approach to improve the efficiency of the CO₂RR processes [3]. In fact, the formation of hybrid materials combining heterogeneous Cu-based nanoreactors with organic or metal-organic frameworks allowed to tune stability of key reaction intermediates, enhancing selectivity towards some specific product [4].

In this work, we developed hybrid molecular-heterogeneous Cu-based nanomaterials for CO₂RR, with the aim of tunning the selectivity of the nanostructured Cu catalysts by combining them with a purely organic molecularly defined polymer. The design of these systems is based on a novel strategy, whereby cuprous oxide (Cu₂O) nanoparticles with a well-defined cubic geometry are used as both, templates and catalyst, for an in-situ polymerization reaction based on azide-alkyne ‘’click’’ reaction between the molecular building blocks. The catalytic performances of the hybrid nanomaterials were tested in a H-type electrochemical cell setup with an online gas-chromatographic quantification analysis (NMR was used for the liquid quantification analysis) and found to be efficient electrocatalysts for CO₂RR obtaining a mixture of C₁-C₂gaseous products (primarily CO, C₂H₄, CH₄ in addition to H₂) and C₁-C₃liquids products (primarily C₂H₆O and CHOO^-) in neutral pH electrolyte.

References:

[1] Franco, F.; Rettenmaier, C.; Jeon, H. S.; Cuenya, B. Transition metal-based electrochemical CO2 reduction: from atoms and molecules to nanostructured materials. Chem. Soc. Adv., 2020, 49, 6884.

[2] Kuhi, K. P.; Cave, E. R.; Abram, D. N.; Jaramillo, T. F. New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces. Energy Environ. Sci., 2012, 7050-7059.

[3] Nam , D.-H.; De Luna, P.; Rosas-Hernández , A.; Thevenon, A.; Li, F.; Agapie, T.; Peters, J. C.; Shekhah, O.; Eddaoudi, M.; Sargent, E. H.; Molecular enhancement of heterogeneous CO2 reduction, Nature Materials, 2020, 19, 266

[4] Li, F.; Wang, Z.; Li, J.; Nam, D. H.; Lum, Y.; Luo, M.; Wang, X.; Ozden, A.; Hung, S. F.; Chen, B.; Wang, Y.; Wicks, J.; Xu, Y.; Li, Y.; Gabardo, C. M.; Dinh, C. T.; Wang, Y.; Zhuang, T. T.; Sinton, D.; Sargent, E. H. Cooperative CO2-to-ethanol conversion via enriched intermediates at molecule–metal catalyst interfaces. Nature Catalysis, 2020, 3, 75-82

Acknowledgements:

J.M.B. thanks to ICIQ Master Projects Fellowship Programme, F.F. thanks MCIN/AEI/10.13039/501100011033 for a Juan de la Cierva-Incorporación fellowship (IJC2019-042363-I). E.P.-G. acknowledges financial support from MINECO (project PID2019-109389RB-I00), SGR-AGAUR 2017SGR00978, ICIQ, CERCA, and ICREA.

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