Rational Design of Peroxymonosulfate Activation and Photoinduced Catalysis Tandem Systems for Artificial Conversion of Solar Light to Chemical Energy
Notice bibliographique
Résumé
It has been known that dedicated photoinduced catalysis over artificial functional nanostructures and/or combined with effective peroxymonosulfate (PMS) activations toward highly effective greener synthesis and/or environmental remediation have been well recognized to be one of the best options for efficiently exploiting solar light to convert into chemical fuel and energy. Novel ZnxCu1–xFe2O4 (0 ≤ x ≤ 1) hierarchical yolk–shell hollow nano-microspheres/PMS/Vis (ZCF/PMS/Vis) tandem systems with remarkable light harvesting capability and superior environmental catalytic activity toward elimination of antibiotic enrofloxacin up to 90.5% removal efficiency have been successfully designed and fabricated via combined solvothermal strategy and morphologically conserved sintering in this current work. The physicochemical characteristics, diverse structures including the spinel crystal structures, hierarchical nano-microstructure, and internal correlations of structure-dependent properties, and the catalytic reaction mechanism in terms of the synergetic effect between instant PMS activation and dedicated photoinitiated catalysis have been methodically inspected and thoroughly illustrated by a variety of in/ex situ physicochemical ways, and the diverse microstructures including solid microspheres with villiform surfaces, YSHMs composed of exquisite particles, and YSHM alternative formation of diverse microstructures could be ultimately tailored and formed. ZCF YSHMs exhibit higher efficiency of both dedicated catalysis and spatial charge separations owing to their physicochemical characteristics and surface structures, namely, more surface oxygen vacancies, highest specific surface area, and interior structures. Specifically, as confirmed by primary combined characterizations, namely, room-temperature Mössbauer, in situ spin-trap EPR, SPV, ns-TAS, and in situ Raman and sequential investigations, the primary reactive oxygen species were deemed to be SO4·– and ·OH radicals, which generated instantly and simultaneously through surface covalent Cu2+ ions. Sequential-derived Cu(II)/Cu(III)/Cu(II) redox cycling initiated PMS activations and photoinitiated catalysis, and the superior catalytic performance as derived from ZCF HYSHM hierarchical-structured spinels could be primarily attributed to the diverse bulk and surface structures, highly efficient photonic energy harvesting, spatial charge separations and surface–interfacial transfers, more surface oxygen vacancies, and crucial reactive species including SO4·– and ·OH generations with long radical lifetimes up to 14.57 μs. The work could bring a brand new and deep insight into further understanding of both the intrinsic spinel structural influence factors governing the catalytic properties and the synergetic effect between instant PMS activation and simultaneous photoinitiated catalysis at the molecular level, which would be very beneficial for mimicking the natural photosynthetic solar energy harness system with marvelous featured properties in both environmental elimination and solar energy conversions.
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Prédiction distillée sur la base complète
Imitation des enseignantsNi prévalence calibrée, ni vérité terrain. Validation humaine à venir. Apprise à partir de 10 348 étiquettes directes de Codex et de 10 348 étiquettes directes de Gemma. Le mode candidate est l'union des têtes enseignantes seuillées; le consensus est leur intersection. Ces sorties portent le statut machine_predicted_unvalidated et ne sont ni des étiquettes humaines ni des étiquettes directes de modèles de pointe.
Scores Codex et Gemma par catégorie
| Catégorie | Codex | Gemma |
|---|---|---|
| Métarecherche | 0,000 | 0,000 |
| Méta-épidémiologie (sens strict) | 0,000 | 0,000 |
| Méta-épidémiologie (sens large) | 0,000 | 0,000 |
| Bibliométrie | 0,000 | 0,000 |
| Études des sciences et des technologies | 0,000 | 0,000 |
| Communication savante | 0,000 | 0,000 |
| Science ouverte | 0,000 | 0,000 |
| Intégrité de la recherche | 0,000 | 0,000 |
| Charge utile insuffisante (le modèle a refusé de juger) | 0,000 | 0,000 |
Scores machine (provisoires)
Les deux têtes enseignantes du modèle étudiant, lues sur ce travail. Un score ordonne la base pour la relecture; il n'affirme jamais une catégorie, et le statut de validation accompagne chaque rangée tel quel.
Scores de référence d'un modèle non mature (critères de maturité non atteints, 7 itérations). Un score ordonne; il n'affirme jamais une catégorie.
score_only:v0-immature-baseline · tel quel depuis la passe de notation : score_only signifie que le nombre peut ordonner les travaux, et qu'aucune étiquette de catégorie n'en découleClassification
machine, non validéePrédiction automatique; un appel candidat d’une seule tête enseignante, pas un consensus.
Le détail, modèle par modèle et score par score, se trouve en fin de page sous « Comment cette classification a été obtenue ».