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Record W4390405115 · doi:10.1021/jacs.3c12438

Interrupted Homolytic Substitution Enables Organoboron Compounds to Inhibit Radical Chain Reactions Rather than Initiate Them

2023· article· en· W4390405115 on OpenAlexafffund
Zijun Wu, Robynne Vlaming, Michael Donohoe, Derek A. Pratt

Bibliographic record

VenueJournal of the American Chemical Society · 2023
Typearticle
Languageen
FieldChemistry
TopicRadical Photochemical Reactions
Canadian institutionsUniversity of Ottawa
FundersNatural Sciences and Engineering Research Council of CanadaCanada Foundation for Innovation
KeywordsChemistryHomolysisAutoxidationRadicalTetracoordinateAlkylRadical substitutionPhotochemistryOrganic chemistry

Abstract

fetched live from OpenAlex

The reactions of organoboranes with peroxyl radicals are key to their use as radical initiators for a vast array of radical chain reactions, particularly at low temperatures where high stereoselectivity or regioselectivity is desired. Whereas these reactions generally proceed via concerted homolytic substitution (S H 2) mechanisms, organoboranes that bear groups that can stabilize tetracoordinate boron radical “ate” complexes (e.g., catecholboranes) undergo this reaction via a stepwise addition/fragmentation sequence and serve as useful stoichiometric alkyl radical precursors. Here we show that arylboronic esters and amides derived from catecholborane and diaminonaphthaleneborane, respectively, are potent radical-trapping antioxidants (RTAs). Mechanistic studies reveal that this is because the radical “ate” complexes derived from peroxyl radical addition to boron are sufficiently persistent to trap another radical in an interrupted S H 2 reaction. Remarkably, the reactivity of these organoboranes as inhibitors of autoxidation was shown to translate from simple hydrocarbons to the phospholipids of biological membranes such that they can inhibit ferroptosis, the cell death modality driven by lipid autoxidation and relevant in neurodegeneration and other major pathologies. The unique mechanism of these organoboranes is one of only a handful of RTA mechanisms that are not based on H-atom transfer processes and provide a new dimension to boron chemistry and its applications.

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)0.000
metaresearch head score (Gemma)0.001
Version: codex-gemma-dda1882f352aValidation 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 score0.004
Threshold uncertainty score0.832

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.001
Bibliometrics0.0000.001
Science and technology studies0.0000.001
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.001
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 head0.025
GPT teacher head0.273
Teacher spread0.249 · 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.

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

Citations5
Published2023
Admission routes2
Has abstractyes

Explore more

Same venueJournal of the American Chemical SocietySame topicRadical Photochemical ReactionsFrench-language works237,207