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| Home > Articles > Published articles > Supramolecular interaction of a molecular catalyst with a polymeric carbon nitride photoanode enhances photoelectrochemical activity and stability at neutral pH |
(Universitat Rovira i Virgili) (Universitat Politècnica de València) (Institut Català d'Investigació Química-ICIQ) (University of the Negev) (Institut Català d'Investigació Química-ICIQ) (Universitat Politècnica de València) (Institut Català d'Investigació Química-ICIQ) (Universitat Autònoma de Barcelona. Departament de Química) (University of the Negev)
| Date: | 2024 |
| Abstract: | Polymeric carbon nitride (CN) emerged as an alternative, metal-free photoanode material for water-splitting photoelectrochemical cells (PECs). However, the performance of CN photoanodes is limited due to the slow charge separation and water oxidation kinetics due to poor interaction with water oxidation catalysts (WOCs). Moreover, operation under benign, neutral pH conditions is rarely reported. Here, we design a porous CN photoanode connected to a highly active molecular Ru-based WOC, which also acts as an additional photo-absorber. We show that the strong interaction between the π-system of the heptazine units within the CN with the CH groups of the WOC's equatorial ligand enables a strong connection between them and an efficient electronic communication path. The optimized photoanode exhibits a photocurrent density of 180 ± 10 μA cm -2 at 1. 23 V vs. the reversible hydrogen electrode (RHE) with 89% faradaic efficiency for oxygen evolution with turnover numbers (TONs) in the range of 3300 and a turnover frequency (TOF) of 0. 4 s -1, low onset potential, extended incident photon to current conversion, and good stability up to 5 h. This study may lead to the integration of molecular catalysts and polymeric organic absorbers using supramolecular interactions. Supramolecular interaction of a Ru oligomeric catalyst with polymeric carbon nitride forms CN-Ru hybrid system, achieving high photoelectrochemical water-splitting activity, enhanced stability, and >89% faradaic efficiency for O at neutral pH. |
| Grants: | European Commission 849068 Agencia Estatal de Investigación PRE2020-093789 Agencia Estatal de Investigación PRE2020-093521 Agencia Estatal de Investigación PID2020-112806RB-I00 Agencia Estatal de Investigación CEX2019-000925-S Agencia Estatal de Investigación CEX-2021-001230-S Agencia Estatal de Investigación PDI2021-0126071-OB-CO21 Agencia Estatal de Investigación RYC2021-031006-I Agencia Estatal de Investigación PID2022-141099OA-I00 Agencia Estatal de Investigación PID2022-140143OB-I00 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-1631 |
| Rights: | Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original.  |
| Language: | Anglès |
| Document: | Article ; recerca ; Versió publicada |
| Published in: | Chemical science, Vol. 15 (September 2024) , p. 16546-16553, ISSN 2041-6539 |
