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Record W2095085213 · doi:10.1021/jp801023v

Free Radical Formation in Supercritical CO<sub>2</sub>, Using Muonium as a Probe and Implication for H Atom Reaction with Ethene

2008· article· en· W2095085213 on OpenAlexaff
Philip Cormier, Donald J. Arseneau, Jean‐Claude Brodovitch, Jean Michel P. Lauzon, Becky Taylor, Khashayar Ghandi

Bibliographic record

VenueThe Journal of Physical Chemistry A · 2008
Typearticle
Languageen
FieldEnergy
TopicCO2 Reduction Techniques and Catalysts
Canadian institutionsSimon Fraser UniversityMount Allison UniversityTRIUMF
Fundersnot available
KeywordsSupercritical fluidChemistryMuoniumHyperfine structureRadicalPhotochemistryReactivity (psychology)Radical disproportionationMethyl radicalPhysical chemistryOrganic chemistryAtomic physicsCatalysis

Abstract

fetched live from OpenAlex

This report presents the first observation of an alkyl radical in supercritical CO(2) by any magnetic resonance technique. Muoniated ethyl radical has been detected in muon-irradiated supercritical CO(2) solutions. In the presence of a low concentration of ethene in supercritical CO(2), it is found that the addition of muonium to ethene is the only reaction channel, and that the yield of this process is enhanced compared to conventional solvents. The temperature dependence of the hyperfine coupling constants of the ethyl radical suggests that at a density of 0.3 g/cm(3) both the rotational motion of the methyl group and the electronic structure of the radical are similar to those in the gas phase, and therefore that the local environment around the ethyl radical is similar to the gas phase under these conditions. At higher densities, however, there is a remarkable and unexpected density dependence of the hyperfine coupling constant of the ethyl radical, which has never been observed in any environment. In this regime, the density dependence suggests that supercritical CO(2) has a significant effect on the electronic structure of the free radical. Thus, changing the density of CO(2) offers a possible means of tuning the radical reactivity. In addition, at a density of close to 0.4 g/cm(3), CO(2) molecules cluster around the ethyl radical, and this increases the local density around the ethyl radical by a factor of ~1.5.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame machine prediction

Teacher imitation

Not 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.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: metacan-v3-hybrid-931329e0061cValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.001
Threshold uncertainty score0.003

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0010.000

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.

Opus teacher head0.016
GPT teacher head0.266
Teacher spread0.251 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designBench or experimental
Domainnot available
GenreEmpirical

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".

Quick stats

Citations12
Published2008
Admission routes1
Has abstractyes

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