Mechanism of Aqueous-Phase Ozonation of S(IV)
Bibliographic record
Abstract
The ozonation of dissolved sulfur dioxide is an important route for sulfate formation, especially in fog and cloud droplets of high pH. However, little is known about the detailed chemical mechanism of this process. We have mapped out the fate of aqueous SO(2) in the presence of ozone by use of density functional theory (DFT) calculations in solution (via the polarized continuum model, PCM), including up to two explicit water molecules. The calculations predict that the hydrolysis of SO(2).H(2)O, although possessing a barrier, is still more energetically favorable than its ozonation. The ozonation of HOSO(2)(-) and SO(3)(2)(-) proceeds without barriers and gives S(VI) products that are more stable than the reagents by 77.1 and 88.6 kcal/mol, respectively. By comparing our calculated pH dependence of the ozonation kinetics to those determined experimentally, we conclude that, despite a high calculated energy barrier to the ozonation of sulfonate (HSO(3)(-)), it is the dominant form of S(IV) in solutions of neutral pH and is the species through which ozonation occurs.
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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 | 0.001 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.002 | 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".