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Molecular triad containing a TEMPO catalyst grafted on mesoporous ITO electrode as photoelectrocatalytic anode for visible light-driven alcohol oxidation

Abstract : Photoelectrochemical cell based on a semiconductor is among the most studied approach for artificial photosynthesis. Here, we investigated a recent concept based on the immobilization, on a mesoporous conducting ITO electrode (nano-ITO), of a molecular triad. The triad NDADI-P-Ru-TEMPO contained a ruthenium tris-bipyridine complex (Ru) as photosensitizer, which was connected in one end to 2,2,6,6-tetramethyl-1-piperidine N-oxyl (TEMPO) as alcohol oxidation catalyst, and in the other end to the electron acceptor naphthalene-dicarboxyanhydride-dicarboximide (NDADI). Light irradiation of the molecular triad (NDADI-P-Ru-TEMPO) grafted to nano-ITO performs selective oxidation of paramethoxy benzylalcohol (MeO-BA) to para-methoxy benzaldehyde in a carbonate buffer (pH = 10) with a TON of  150 after 1 hour of photolysis at a bias of 0.4 V vs. SCE and the faradaic efficiency (FE) is found to be of 805%. The photophysical study indicates that the photoinduced electron transfer from the Ru complex to NDADI is a slow process and must compete with direct electron injection into ITO to have a better performing system. This work sheds some light on some of the important features to design more efficient molecular systems for the preparation of photoelectrocatalytic cell based on the immobilized on conducting electrode of a "Catalyst-Dye-Acceptor" molecular array.
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https://hal-cnrs.archives-ouvertes.fr/hal-03419882
Contributor : Stéphane Diring Connect in order to contact the contributor
Submitted on : Monday, November 8, 2021 - 5:32:07 PM
Last modification on : Tuesday, November 9, 2021 - 4:04:16 AM

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Palas Baran Pati, Mohamed Abdellah, Stéphane Diring, Leif Hammarström, Fabrice Odobel. Molecular triad containing a TEMPO catalyst grafted on mesoporous ITO electrode as photoelectrocatalytic anode for visible light-driven alcohol oxidation. ChemSusChem, ChemPubSoc Europe/Wiley, 2021, 14 (14), pp.2902-2913. ⟨10.1002/cssc.202100843⟩. ⟨hal-03419882⟩

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