Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.143
Publication date: 22nd December 2022
Porphyrins have been actively investigated as oxygen evolution reaction (OER) catalysts, yet only a few studies refer to their integration into electrode devices as heterogeneous catalysts [1-2], mainly due to processability constraints. Moreover, the catalytic activity of porphyrin films can be substantially improved by their modification in the form of conjugated polymers. The enhanced conductivity of metalloporphyrin conjugated polymers, resulting from the extended delocalization of π-electrons in the conjugated system, may promote a faster charge transfer to the active sites, improving the catalytic performance. Recently, our group developed a methodology allowing the straightforward preparation of fused metalloporphyrins conjugated polymers thin films over a wide variety of substrates, based on the oxidative chemical vapour deposition (oCVD) [3,4]. In this way, a new venue for the study of the electrocatalytic activity of fused metalloporphyrin conjugated polymers bearing different metal centres and substituents was opened. Consequently, we have investigated the electrocatalytic activity of Ni(II) and Co(II) fused porphyrins conjugated polymers on FTO substrates towards the OER. We found out that there is a significant role of the direct fusion reaction to form organized electrocatalysts able to operate at lower overpotentials than the monomeric counterparts, resulting in enhanced electrocatalytic performance. Nonetheless, previous reports on Ni and Co complexes, including porphyrins, have demonstrated the decomposition of the molecular matrix to form a material thin film[2,5], possibly a metal oxide specie, acting as the true catalyst for water oxidation at the electrode surface. Therefore, we have conducted a deep-through investigation of the possible conversion of fused metalloporphyrin polymers into a material catalyst, using the combination of structural and compositional analysis with theoretical studies. We pay special attention to the role of polymerization and the presence of substituents of different natures on the transformation kinetics and resulting electrocatalytic activity.
European Research Council (ERC) through the ERC Consolidator Grant project CLEANH2 (grant agreement no. 865985)
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