Structural Variation and Charge-Transfer Dynamics of Protonated β-Ketoenamine-Linked Covalent Organic Framework for Boosted Photocatalytic H 2 Evolution
Rattachement africain : cn, us. Niveau de preuve : code pays fourni par la source.
Le résumé fourni par la source
The surface characteristics of covalent organic framework (COF) photocatalysts can be intentionally altered by the protonated treatment, a straightforward postmodification process. This study provides some insights into the specific variation in crystallinity, microstructures, chemical bonds, charge-transfer dynamics mechanism, electronic distribution, and activation energy resulting from the introduction of protons in a β-ketoenamine-linked COF (TpPa-1). It demonstrates that the introduced protons are attached to the –NH of β-ketoenamine groups to form the –NH···H + groups. Moreover, it is found that the protonated TpPa-1 treated with 0.5 M HOAc solution exhibits a photocatalytic hydrogen evolution rate of 0.238 mmol h –1 in 100 mL ascorbic acid solution at the stationary point with the photocatalyst concentration of 400 mg L –1 without any cocatalysts under visible-light irradiation, equivalent to the mass-normalized value of 5.95 mmol h –1 g –1, which is about 40 and 20 times higher than that of pristine TpPa-1 and TpPa-1 treated with HCl solution, respectively. The isotopic labeling measurement demonstrated that both H 2 O and ascorbic acid molecules served as the sources of evolved H 2 . Furthermore, the significantly improved photocatalytic hydrogen evolution performance could be associated with the introduced protons and the acid–base adducts presented in the sample of TpPa-1-HOAc, as demonstrated by X-ray absorption near-edge spectra (XANES), which contributed to the promoted charge separation efficiency as well as the longer lifetime of photoexcited electrons. Additionally, density functional theory (DFT) calculations reveal that the protonated TpPa-1-HOAc shows special electron density redistribution and favorable Gibbs free energy (Δ G H* ), which contributed to the significantly boosted photocatalytic H 2 evolution performance.
Ce résumé expose les affirmations des auteurs. BNTIC ne l’interprète pas comme une validation indépendante des résultats.
Le contrôle bibliographique ouvert
DOI retrouvé dans Crossref DOI retrouvé, mais le titre doit être comparé manuellement.
- Titre Crossref
- Structural Variation and Charge-Transfer Dynamics of Protonated β-Ketoenamine-Linked Covalent Organic Framework for Boosted Photocatalytic H <sub>2</sub> Evolution
- Date Crossref
- 18/10/2025
- Éditeur
- American Chemical Society (ACS)
- Type
- journal-article
Ce recoupement confirme des métadonnées liées au DOI. Il ne confirme ni la méthode ni les conclusions de l’étude, et il ne compte pas comme une seconde source scientifique indépendante.
Où se fait cette recherche
-
Yancheng Institute of Technology pays non établi dans la noticeUniversité ou école supérieure
-
Jiangsu Provincial Key Laboratory of New Environmental Protection pays non établi dans la noticeStructure de recherche
-
Fairfield University pays non établi dans la noticeUniversité ou école supérieure
-
East China University of Science and Technology pays non établi dans la noticeUniversité ou école supérieure
-
Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province pays non établi dans la noticeStructure de recherche
-
College of Arts and Sciences Department of Chemistry & Biochemistry pays non établi dans la noticeUniversité ou école supérieure
-
School of Chemistry and Molecular E State Key Laboratory of Green Chemical Engineering and Industrial Catalysis pays non établi dans la noticeUniversité ou école supérieure
Yancheng Institute of Technology, Jiangsu Provincial Key Laboratory of New Environmental Protection et Fairfield University, avec 4 autres affiliations.
Une affiliation ne permet pas de déduire la nationalité d’un auteur.