Rational Design of Peroxymonosulfate Activation and Photoinduced Catalysis Tandem Systems for Artificial Conversion of Solar Light to Chemical Energy
Bibliographic record
Abstract
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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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one teacher head, not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".