Academic Journal
The Power of Catalytic Centers and Ascorbate in Boosting the Photocatalytic Hydrogen Evolution Performance of TpDTz 2D-COF
| Τίτλος: | The Power of Catalytic Centers and Ascorbate in Boosting the Photocatalytic Hydrogen Evolution Performance of TpDTz 2D-COF |
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| Συγγραφείς: | Reyes-Mesa, David, Sarró, Pau, Freixanet Gustà, Muriel, Jiménez-Solano, Alberto, Das, Saunak, Biswal, Bishnu P., Vignolo-González, Hugo A., Velasco-Garcia, Laura, Llobet Dalmases, Antoni, Bastús, Neus G., Puntes, Víctor, Vallribera, Adelina, Pleixats, Roser, Granados, Albert, Lotsch, B.V., Gimbert-Suriñach, Carolina |
| Έτος έκδοσης: | 2026 |
| Συλλογή: | Universitat Autònoma de Barcelona: Dipòsit Digital de Documents de la UAB |
| Θεματικοί όροι: | American Chemical Society, Catalytic centre, Covalent organic frameworks, Donor groups, Electron donors, Electron-acceptor, Performance, Photocatalytic hydrogen evolution, Platinum nanoparticles, Power |
| Περιγραφή: | Altres ajuts: acords transformatius de la UAB ; The photocatalytic hydrogen evolution activity of a model 2D covalent organic framework (TpDTz) containing a thiazolo[5,4-d]thiazole (DTz) electron acceptor and triformylphloroglucinol (Tp) electron donor groups is enhanced by combining it with well-defined catalytic centers and suitable sacrificial electron donors. Platinum nanoparticles (PtNPs) with an average diameter of 2.7 ± 0.4 nm achieve rates up to 106 000 μmol H g h (5% Pt w/w). The best system requires the use of ascorbic acid/ascorbate buffer, which has been demonstrated to enhance the photoluminescence of TpDTz by forming aggregates while efficiently extracting charges from the excited TpDTz (TpDTz*). The productive charge extraction by the PtNPs from TpDTz* is also supported by steady state and time-resolved photoluminescence studies. All these factors combined with the high catalytic activity of PtNPs catalytic centers lead to the high performance of the overall system. In addition, a noble metal-free molecular catalyst based on a tetraazamacrocyclic cobalt complex has been identified as a good alternative catalyst candidate, efficiently quenching TpDTz photoluminescence. Under optimal conditions, the cobalt-based system achieves catalytic rates of 10 400 μmol H g h (1% Co w/w) which is only three times slower than the noble metal-based PtNPs system (1% Pt w/w, 28 300 μmol H g h). By using controlled catalytic centers, it was possible to identify the factors limiting the hydrogen evolution photocatalytic activity of TpDTz allowing one to minimize undesired pathways and enhancing its performance by 2 orders of magnitude. |
| Τύπος εγγράφου: | article in journal/newspaper |
| Περιγραφή αρχείου: | application/pdf |
| Γλώσσα: | English |
| ISBN: | 978-2-02-112491-0 2-02-112491-6 |
| ISSN: | 15205126 |
| Relation: | Agencia Estatal de Investigación PID2021-128496OB-I00; Agencia Estatal de Investigación PID2021-124916NB-I00; Agencia Estatal de Investigación PID2023-148967OB-C21; Ministerio de Ciencia e Innovación RED2022-134287-T; Generalitat de Catalunya 2021/SGR-00064; Generalitat de Catalunya 2021/SGR-00878; Generalitat de Catalunya 2023/CLIMA-00036; Ministerio de Ciencia, Innovación y Universidades CEX2024-001469-S; Agencia Estatal de Investigación PID2022-140143OB-I00; Journal of the American Chemical Society; Vol. 148, Num. 1 (December 2026), p. 1316-1328; https://ddd.uab.cat/record/324990; urn:10.1021/jacs.5c17806; urn:oai:ddd.uab.cat:324990; urn:scopus_id:105027588686; urn:articleid:15205126v148n1p1316 |
| Διαθεσιμότητα: | https://ddd.uab.cat/record/324990 |
| Rights: | open access ; 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, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original. ; https://creativecommons.org/licenses/by/4.0/ |
| Αριθμός Καταχώρησης: | edsbas.20594EAD |
| Βάση Δεδομένων: | BASE |
| ISBN: | 9782021124910 2021124916 |
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| ISSN: | 15205126 |