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Record W4396917215 · doi:10.1002/chem.202400788

Unusual Photochemistry in Aromatic Dithioimides: Quantitative Thione Reduction Promoted by Ether Solvents

2024· article· en· W4396917215 on OpenAlexafffund
Steven Mauries, Taylor O. Hope, Katie M. Psutka, Joshua LeDrew, Meghan Heer, Emma Guillet, Pedram Zand, Kenneth E. Maly, Mathieu Frenette

Bibliographic record

VenueChemistry - A European Journal · 2024
Typearticle
Languageen
FieldChemistry
TopicSulfur-Based Synthesis Techniques
Canadian institutionsWilfrid Laurier UniversityUniversité du Québec à Montréal
FundersNatural Sciences and Engineering Research Council of Canada
KeywordsChemistryPhotochemistryEtherSinglet oxygenOxygenSolventMethyleneYield (engineering)Organic chemistry

Abstract

fetched live from OpenAlex

Abstract We report a mechanistic investigation of an aromatic dithioimide ( 2SS ) displaying puzzling yet efficient photochemistry in ether solvents. Perplexingly, 2SS dissolved in ether solvents in a sealed and degassed vial was photochemically converted to the corresponding diimide ( 2OO ), as determined by 1 H NMR following product extraction. With no external sources of oxygen in the sample, could the oxygen in 2OO be from the ether itself? To study this unprecedented proposition, we attempt to uncover the ether's involvement in this reaction. As seen by laser‐flash photolysis, 2SS appears to first react with the solvent from its singlet excited state. Following the reaction by NMR under rigorously oxygen‐ and water‐free conditions led to the identification of a photoreductive pathway that quantitatively transformed one thione into a methylene to yield 2SH 2 . Subsequent oxidation of 2SH 2 or irradiation of 2SS under air proved that molecular oxygen was indeed necessary to observe an oxidative pathway leading to 2OO , ruling out the initially proposed involvement of an ether oxygen. An explanation of 2SS desulfurization was further revealed through the study of solvent by‐products by GC‐MS analysis. Supported by DFT calculations, a mechanism is proposed to involve a chain reaction initiated by photochemically generated ether radical.

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 distilled prediction

Teacher imitation

Not 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.

metaresearch head score (Codex)0.001
metaresearch head score (Gemma)0.001
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow), Insufficient payload (model declined to judge)
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 score0.028
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.001
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 science0.0010.000
Research integrity0.0000.002
Insufficient payload (model declined to judge)0.0020.000

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 head0.021
GPT teacher head0.275
Teacher spread0.254 · 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 teacher head, not a consensus.

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

Citations0
Published2024
Admission routes2
Has abstractyes

Explore more

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