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This work was financially supported by Research Project TED2021-129886B-C43, TED 2021-129886B-C42 and TED2021-132790B-I00 granted by MCIN/AEI/10.13039/501100011033 and the European Union NextGeneration EU/PRTR; and Research Project PID2022-138908NB-C33, PID 2022-138908NBC31 and PID2022-140142OB-I00 granted by MCIN/AEI/10.13039/501100011033/ and FEDER A way to make Europe and the Spanish MICINN (PDC 2022-133498-I00). J. L. S. acknowledges the MICIIN for the REDES project "RED2022-134503-T". J. L.-F. acknowledges Fundacion Ramon Areces for the project ElectroFuel and Spanish MCINN for PDC2022-133451-I00. JIM acknowledges financial support from Spanish MCINN (grants PID2020-113142RB-C21, PLEC2021-007906 and TED2021-129416A-I00), Comunidad de Madrid (grant Y2020/NMT-6469), and CSIC (grant BILAT23033). ES and EGM acknowledge financial support from Spanish MICINN (grant PID2021-123295NB-I00). J. L.-F. and G. C. D. B. also acknowledge the financial support of the ICIQ Foundation, the CERCA Program/Generalitat de Catalunya, MCIN through Severo Ochoa Excellence Accreditation 2020-2023 (CEX2019-000925-S, MIC/AEI), AGAUR (2021 SGR 01260), and Excellence in R&D (CEX 2018-000805-M). This work was also supported by the "Maria de Maeztu" Programme for Units of Excellence in R&D (CEX 2018-000805-M) and the Comunidad de Madrid (MAD2D-CM and TEC-2024/ECO-332) and MICINN (Planes complementarios, Materiales Avanzados). FZ also acknowledges support from the European Innovation Council under grant Agreement 101047081 (EVA).

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Post-synthetic modification of covalent organic frameworks with active manganese centers for electrocatalytic CO2 reduction in water

Publicated to:Journal of Materials Chemistry A. 13 (2): 1142-1152 - 2024-11-26 13(2), DOI: 10.1039/d4ta02807d

Authors: Gala, Elena; Bandomo, Geyla C Dubed; Bandomo, Geyla C Dubed; Vettori, Mattia; Royuela, Sergio; Martinez-Fernandez, Marcos; Martinez, Jose I; Martinez, Jose I; Salagre, Elena; Michel, Enrique G; Michel, Enrique G; Zamora, Felix; Lloret-Fillol, Julio; Segura, Jose L; Segura, Jose L

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Abstract

The development of effective catalysts for the CO2 reduction reaction (CO2RR) is essential for transforming atmospheric CO2 into valuable chemical scaffolds. While numerous catalysts have been developed for the CO2RR, few are suitable for use in aqueous systems due to inherent design challenges. In this context, Covalent Organic Frameworks (COFs) have emerged as promising materials for the CO2RR in water, offering potential solutions to these challenges. Thanks to their porosity, high surface area and crystalline structure, COFs are excellent hosts for single-atom catalysts (SACs), enabling the immobilization of high-value species and their utilization in heterogeneous catalytic processes. For this reason, we have explored the catalytic activity of a terpyridine-manganese complex integrated into a COF lattice, which was successfully synthesized and characterized, confirming the presence of the metal ion in the material with spectroscopic techniques such as XPS and EDS. This new material has proved to be an active heterogeneous catalyst for the CO2RR in water as solvent, achieving a faradaic yield of 42% for CO at 300 mV overpotential and 16% for formate when 600 mV was applied. Furthermore, an ab initio theoretical study was performed to provide a plausible mechanism of the CO2RR to elucidate the CO evolution pathway.

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