Gas-Phase HO<sup>•</sup>-Initiated Reactions of Elemental Mercury: Kinetics, Product Studies, and Atmospheric Implications
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Bibliographic record
Abstract
Mercury is an environmentally volatile toxic fluid metal that is assumed to have a long atmospheric residence time and hence is subject to long-range transport. The speciation and chemical transformation of mercury in the atmosphere strongly influences its bioaccumulation potential in the human food chain as well as its global cycling. To investigate the oxidation of Hg0 by HO, the dominantdaytime atmospheric oxidant, we performed kinetic and product studies over the temperature range 283-353 K under near atmospheric pressure (100+/-0.13 kPa) in air and N2 diluents. Experiments were carried out by the relative rate method using five reference molecules and monitored by gas chromatography with mass spectroscopic detection (GC-MS). The HO were generated using UV photolysis of isopropyl nitrite at 300 < or = lambda < or = 400 nm in the presence of NO. The room-temperature rate constant was found to be (9.0+/-1.3) x 10(-14) cm3 molecule(-1) s(-1). The temperature dependence of the reaction can be expressed as a simple Arrhenius expression (in unit of 10(-14) cm3 molecule(-1) s(-1)) using ethane as the reference molecule: kHg + HO = 3.55 x 10(-14) exp((294+/-16)/T). The major reaction product, HgO, was identified in the gaseous form, as aerosols and as deposits on the container walls, using chemical ionization mass spectrometry (CI-MS), electron impact mass spectrometry (EI-MS), GC-MS, and cold vapor atomic fluorescence spectrometry (CVAFS). Experimental results reveal that ca. 6% of the reaction products were collected on a 0.2 microm filter as suspended aerosol, ca. 10% were in the gaseous form, and about 80% were deposited on the reaction vessel wall. The potential implications of our results in the understanding of tropospheric mercury transformation are herein discussed.
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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 | 0.001 |
| Science and technology studies | 0.001 | 0.007 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.001 |
| 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 it