Supramolecular interaction of a molecular catalyst with a polymeric carbon nitride photoanode enhances photoelectrochemical activity and stability at neutral pH
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| dc.contributor.author | Mondal, Sanjit
|
es_ES |
| dc.contributor.author | Salati, Martina
|
es_ES |
| dc.contributor.author | Nicaso, Marco
|
es_ES |
| dc.contributor.author | Albero-Sancho, Josep
|
es_ES |
| dc.contributor.author | Segado-Centellas, Mireia
|
es_ES |
| dc.contributor.author | Michael Volokh
|
es_ES |
| dc.contributor.author | Bo, Carles
|
es_ES |
| dc.contributor.author | García Gómez, Hermenegildo
|
es_ES |
| dc.contributor.author | Gil-Sepulcre, Marcos
|
es_ES |
| dc.contributor.author | Llobet, Antoni
|
es_ES |
| dc.contributor.author | Menny, Shalom
|
es_ES |
| dc.date.accessioned | 2024-11-06T19:19:34Z | |
| dc.date.available | 2024-11-06T19:19:34Z | |
| dc.date.issued | 2024-09 | es_ES |
| dc.identifier.issn | 2041-6520 | es_ES |
| dc.identifier.uri | http://hdl.handle.net/10251/211453 | |
| dc.description.abstract | [EN] 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 pi-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 mu A 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. | es_ES |
| dc.description.sponsorship | This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant Agreement No. 849068). This work was also partially supported by the Israel Science Foundation (ISF), Grant No. 601/21. MS and MN acknowledge the Ministerio de Ciencia e Innovacion (MICINN) for the grants PRE2020-093789 and PRE2020-093521, respectively. CB gratefully acknowledges MCINN/AEI/10.13039/501100011033 for projects PID2020-112806RB-I00 and CEX2019-000925-S, the ICIQ Foundation and the CERCA program of the Generalitat de Catalunya for funding. HG thanks MICINN (CEX-2021-001230-S and PDI2021-0126071-OB-CO21 funded by MCIN/AEI/10.13039/501100011033), Generalitat Valenciana (Prometeo 2021/038 and Advanced Materials programme Graphica MFA/2022/023 with funding from European Union Next Generation EU PRTR-C17.I1). JA thanks the MICINN for a Ramon y Cajal research associate contract (RYC2021-031006-I funded by MCIN/AEI/10.13039/501100011033 and by "European Union Next Generation EU/PRTR), and acknowledges the financial support (PID2022-141099OA-I00 funded by MCINN/AEI/10.13039/501100011033 and by "European Union Next Generation EU/PRTR). AL acknowledges MICINN through the project PID2022-140143OB-I00, Generalitat de Catalunya for the project 2017 SGR 1631 and Severo Ochoa (CEX2019-000925-S). | es_ES |
| dc.language | Inglés | es_ES |
| dc.publisher | The Royal Society of Chemistry | es_ES |
| dc.relation.ispartof | Chemical Science | es_ES |
| dc.rights | Reconocimiento - No comercial (by-nc) | es_ES |
| dc.subject.classification | QUIMICA ORGANICA | es_ES |
| dc.title | Supramolecular interaction of a molecular catalyst with a polymeric carbon nitride photoanode enhances photoelectrochemical activity and stability at neutral pH | es_ES |
| dc.type | Artículo | es_ES |
| dc.identifier.doi | 10.1039/d4sc04678a | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2020-112806RB-I00/ES/QUIMICA COMPUTACIONAL 4.0 PARA UN DESARROLLO SOSTENIBLE/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-140143OB-I00/ES/CATALIZADORES MOLECULARES REDOX PARA SU APLICACION EN ENERGIA VERDE/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-141099OA-I00/ES/DISEÑO Y PREPARACION DE CATALIZADORES FOTO-TERMICOS PARA LA PRODUCCION DE COMBUSTIBLES SOLARES/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/EC/H2020/849068/EU/Controlled Growth of Lightweight Metal-Free Materials for Photoelectrochemical Cells/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/GC//2017 SGR 1631/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/GVA//PROMETEO%2F2021%2F038/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/GVA//MFA%2F2022%2F023/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/ISF//601%2F21/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/AEI//CEX2019-000925-S/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/AEI//PDI2021-0126071-OB-CO21/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/MICINN//CEX2021-001230-S/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/MICINN//PRE2020-093789/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/MICINN//PRE2020-093521/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/MICINN//PRTR-C17.I1/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/MICINN//RYC2021-031006-I/ | es_ES |
| dc.rights.accessRights | Abierto | es_ES |
| dc.contributor.affiliation | Universitat Politècnica de València. Escuela Técnica Superior de Ingenieros Industriales - Escola Tècnica Superior d'Enginyers Industrials | es_ES |
| dc.contributor.affiliation | Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química | es_ES |
| dc.description.bibliographicCitation | Mondal, S.; Salati, M.; Nicaso, M.; Albero-Sancho, J.; Segado-Centellas, M.; Michael Volokh; Bo, C.... (2024). Supramolecular interaction of a molecular catalyst with a polymeric carbon nitride photoanode enhances photoelectrochemical activity and stability at neutral pH. Chemical Science. https://doi.org/10.1039/d4sc04678a | es_ES |
| dc.description.accrualMethod | S | es_ES |
| dc.relation.publisherversion | https://doi.org/10.1039/d4sc04678a | es_ES |
| dc.type.version | info:eu-repo/semantics/publishedVersion | es_ES |
| dc.relation.pasarela | S\527602 | es_ES |
| dc.contributor.funder | European Commission | es_ES |
| dc.contributor.funder | Generalitat Valenciana | es_ES |
| dc.contributor.funder | Generalitat de Catalunya | es_ES |
| dc.contributor.funder | Israel Science Foundation | es_ES |
| dc.contributor.funder | Centres de Recerca de Catalunya | es_ES |
| dc.contributor.funder | Agencia Estatal de Investigación | es_ES |
| dc.contributor.funder | Ministerio de Ciencia e Innovación | es_ES |
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