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Record W2076026935 · doi:10.1139/v09-080

Rearrangement mechanisms for azoxypyridines and azoxypyridine <i>N</i> -oxides in the 100% H <sub>2</sub> SO <sub>4</sub> region — The Wallach rearrangement story comes full circle

2009· article· en· W2076026935 on OpenAlexafffundvenue
Erwin Buncel, Sam‐Rok Keum, Srinivasan Rajagopal, Robin A. Cox

Bibliographic record

VenueCanadian Journal of Chemistry · 2009
Typearticle
Languageen
FieldChemistry
TopicChemical Reaction Mechanisms
Canadian institutionsThe Scarborough HospitalQueen's University
FundersNational Research Council CanadaNatural Sciences and Engineering Research Council of Canada
KeywordsChemistryReaction rate constantCatalysisReaction mechanismMedicinal chemistryStereochemistryKineticsComputational chemistryOrganic chemistryPhysicsQuantum mechanics

Abstract

fetched live from OpenAlex

Kinetic studies of the Wallach rearrangements of four azoxypyridines, four azoxypyridine N-oxides, and one azoxypyridine N-methiodide have been carried out in the 100% H 2 SO 4 acidity region. For all of the β-isomers in the study the reactions proceeded at a spectrally measurable rate, and the log observed rate constants were found to be linear functions of the log H 3 SO 4 + concentration, as previously found for azoxybenzene itself, suggesting that the reaction mechanism for these substrates is the same as that previously deduced for axozybenzene, i.e., a general-acid-catalysis A-S E 2 process. For the α-azoxypyridines no reaction could be observed at all. The two α-azoxypyridine N-oxides in the study did react, albeit very slowly, but for these two compounds the log observed rate constants were not linear functions of the log H 3 SO 4 + concentration, but were instead found to be linear in the H 0 acidity function, which is known for the 100% H 2 SO 4 acidity region. It follows that the reaction mechanism for these α-isomers is a different one, presumably an A1 process. This mechanism was proposed back in 1963 for azoxybenzene, but has never actually been observed for any substrate before the work reported in this study. Thus, the Wallach rearrangement story can be said to have come full circle.

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)
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 score0.015
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
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 head0.013
GPT teacher head0.213
Teacher spread0.200 · 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

Citations8
Published2009
Admission routes3
Has abstractyes

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