Phase-Migrating Z-Scheme Charge Transportation Enables Photoredox Catalysis Harnessing Water as an Electron Source
Bibliographic record
Abstract
Z-schematic photocatalytic reactions are of considerable interest because of their potential for application to reductive molecular conversions to value-added chemicals using water as an electron source. However, most demonstrations of Z-scheme photocatalysis have been limited to overall water splitting. In particular, it has been basically impossible to couple the reduction of “water-insoluble compounds” with water oxidation by conventional Z-scheme systems in aqueous solution. In this work, an unconventional Z-scheme electron transportation system with a “phase-migrating” redox mediator is constructed that enables photocatalytic conversion of water-insoluble compounds by using water as an electron/proton source. In a dichloroethane (DCE)/water biphasic solution, a molecular Ir(III) complex acts as a photoredox catalyst for the reductive coupling of benzyl bromide by using ferrocene (Fc) as an electron donor in the DCE phase. On the other side, an aqueous dispersion of a Bi 4 TaO 8 Cl semiconductor loaded with a (Fe,Ru)O x cocatalyst photocatalyzed water oxidation using ferrocenium (Fc + ) as an electron acceptor. Because the partition coefficients of Fc + /Fc are significantly different, the Fc + and Fc generated by photoinduced electron transfer in each reaction could be selectively extracted to the opposite liquid phase. Spontaneous phase migration enables direction-selective electron transport across the organic/water interface that connects the reduction and oxidation reactions in the separated reaction phase. Eventually, photocatalytic reductive conversion of “water-insoluble” organic compounds using “water as the electron/proton source” was demonstrated through the step-by-step Z-scheme photocatalysis with the phase-migrating Fc + /Fc electron transportation.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| 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) | 0.001 | 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 source (direct Gemma or distilled Codex), 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".