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Record W4387609159 · doi:10.1021/acscatal.3c03994

Photocatalytic C–S Bond Formation Using <i>N</i>-Thiophthalimide and <i>N-</i>Perthiophthalimide Derivatives

2023· article· en· W4387609159 on OpenAlex

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.
fundA Canadian funder is recorded on the work.

Bibliographic record

VenueACS Catalysis · 2023
Typearticle
Languageen
FieldChemistry
TopicSulfur-Based Synthesis Techniques
Canadian institutionsUniversity of Ottawa
FundersNatural Sciences and Engineering Research Council of CanadaCanada Foundation for InnovationGovernment of Ontario
KeywordsPhotoredox catalysisChemistryReagentRadicalHomolysisCatalysisPhotochemistryPhotocatalysisSubstitution reactionAlkylCombinatorial chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Unsymmetric disulfides are shown to be accessed directly from carboxylic acids or trifluoroborate salts by using N -perthiophthalimide derivatives (Harpp reagents) under photoredox catalysis. While this would appear to involve homolytic substitution of alkyl radicals on the Harpp reagents, the formation of the high-energy phthalimidyl radical renders this reaction prohibitively endergonic. Instead, computations and experiments suggest that the Harpp reagents are reduced in situ to form perthiyl radicals that dimerize to tetrasulfides (RSSSSR), which have previously been demonstrated to undergo radical substitution to give disulfides. Given these results, examples of previously reported radical sulfurations using N -thiophthalimide reagents under photoredox catalysis were investigated. Our results suggest that these reactions are likely to proceed via in situ formation of the corresponding disulfide as the sulfuration reagent rather than direct substitution on the N -thiophthalimide. The implications of these findings for the use of phthalimide (and related) derivatives in photoredox-catalyzed reactions are discussed.

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.

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)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow)
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 score0.004
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.001
Science and technology studies0.0000.000
Scholarly communication0.0000.001
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0000.000

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 head0.037
GPT teacher head0.278
Teacher spread0.242 · 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