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Record W4286219558 · doi:10.26434/chemrxiv-2022-71bzc

A generally applicable quantitative reactivity model for nucleophilic aromatic substitution built from simple descriptors

2022· preprint· en· W4286219558 on OpenAlexafffund
Jingru Lu, Irina Paci, David C. Leitch

Bibliographic record

VenueChemRxiv · 2022
Typepreprint
Languageen
FieldChemistry
TopicChemical Reaction Mechanisms
Canadian institutionsUniversity of Victoria
FundersNatural Sciences and Engineering Research Council of CanadaWestern Canada Research GridCompute CanadaUniversity of Victoria
KeywordsNucleophilic aromatic substitutionChemistryCarbocationRegioselectivityComputational chemistryElectrophileNucleophilic substitutionElectrophilic aromatic substitutionOrganic chemistry

Abstract

fetched live from OpenAlex

We report a multivariate linear regression model able to make accurate predictions for the rate and regioselectivity of nucleophilic aromatic substitution (SNAr) reactions based on the electrophile structure. This model uses a diverse training/test set from experimentally-determined relative SNAr rates between benzyl alcohol and 74 unique electrophiles, including heterocycles with multiple substitution patterns. There is a robust linear relationship between the experimental SNAr free energies of activation and three molecular descriptors that can be obtained computationally: the LUMO energy of the electrophile; the average molecular electrostatic potential (ESP) at the carbon undergoing substitution; and the sum of average ESP values for the ortho and para atoms relative to the reactive center. Despite using only simple descriptors calculated from ground state wavefunctions, this model demonstrates excellent correlation with previously measured SNAr reaction rates, and is able to accurately predict site selectivity for multihalogenated substrates: 91% prediction accuracy across 82 individual examples. The excellent agreement between predicted and experimental outcomes makes this easy-to-implement reactivity model a potentially powerful tool for synthetic planning.

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 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 score0.406
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.001
Meta-epidemiology (narrow)0.0010.001
Meta-epidemiology (broad)0.0010.001
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0010.001
Research integrity0.0010.001
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 head0.075
GPT teacher head0.304
Teacher spread0.228 · 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
Published2022
Admission routes2
Has abstractyes

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