Self-Driven-Formed Cu(III) Enables Rapid Decomplexation of Cu(II)-EDTA in UV/Peroxymonosulfate under Acidic Conditions
Bibliographic record
Abstract
Effective degradation of metal–organic complexes in wastewater remains a pressing challenge due to their strong coordination stability and resistance to oxidation. Conventional advanced oxidation processes (AOPs) often treat such complexes as passive targets, overlooking their intrinsic chemical reactivity. Here, we demonstrate that Cu(II)-EDTA, a representative coordination pollutant, can actively participate in a redox-mediated self-degradation process under UV-activated peroxymonosulfate (UV/PMS) conditions. Experimental and computational evidence reveals a Cu(II)–Cu(I)–Cu(III) transformation pathway, in which the high-valent Cu(III)-oxo species drive hydrogen abstraction and decarboxylation reactions. Acidic pH enhances ligand protonation, weakens coordination bonds, and increases α-C–H lability, thereby accelerating degradation, which does not occur at pH ≥ 7. Electron paramagnetic resonance (EPR), quenching tests, and kinetic modeling confirm the significant contribution of the in situ generation of Cu(III). Density functional theory (DFT) calculations support a mechanism involving Jahn–Teller distortion and spin-density redistribution, promoting the formation of Cu(III)-oxyl intermediates. The UV/PMS system achieves over 90% Cu(II)-EDTA removal in actual electroplating wastewater, demonstrating strong resistance to anions and moderate inhibition by natural organic matter. These findings redefine the role of metal complexes as reactive agents in AOPs and offer a mechanistic foundation for designing pollutant-induced, self-enhanced degradation strategies in engineered water treatment applications.
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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 | 0.001 |
| 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 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".