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Record W3135211133 · doi:10.1002/ejoc.202100093

A DFT Study on the Mechanism and Origin of Regioselectivity in the Rhodium/Diene‐Catalyzed Ring‐Opening Reactions of C1‐Substituted Oxabenzonorbornadienes with Arylboronic Acids

2021· article· en· W3135211133 on OpenAlexaff
Austin Pounder, Fiona Bishop, Leanne D. Chen, William Tam

Bibliographic record

VenueEuropean Journal of Organic Chemistry · 2021
Typearticle
Languageen
FieldChemistry
TopicAsymmetric Hydrogenation and Catalysis
Canadian institutionsUniversity of Guelph
Fundersnot available
KeywordsProtonolysisRegioselectivityChemistryDieneRhodiumTransmetalationRing (chemistry)CatalysisReductive eliminationReaction mechanismDensity functional theoryCombinatorial chemistryMedicinal chemistryComputational chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Abstract The mechanism and the origin of the regioselectivity of the rhodium/diene‐catalyzed ring‐opening reactions of C1‐substituted oxabenzonorbornadienes with arylboronic acids has been examined using hybrid density functional theory (DFT). The overall mechanism for the reaction is considered as a four‐step reaction including transmetalation, carborhodation, β‐oxygen elimination, and protonolysis. The free energy profiles show that the rate‐determining step is involved in the protonolysis step which differs from previous mechanistic studies on metal‐catalyzed ring‐opening reactions of oxabenzonorbornadienes. Additionally, it is theorized the β‐oxygen elimination step is the origin of regioselectivity. DFT calculations predict the formation of the 1,2,4‐trisubstituted naphthalene framework is selective over the 1,1,2‐trisubstituted product, in agreement with experimental observations.

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 machine prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: metacan-v3-hybrid-931329e0061cValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Simulation or modeling · Consensus signal: Simulation or modeling
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.006
Threshold uncertainty score0.018

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0010.000
Meta-epidemiology (broad)0.0010.001
Bibliometrics0.0010.000
Science and technology studies0.0010.000
Scholarly communication0.0010.001
Open science0.0010.000
Research integrity0.0010.001
Insufficient payload (model declined to judge)0.0050.000

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 head0.018
GPT teacher head0.226
Teacher spread0.208 · 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 source (direct Gemma or distilled Codex), not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designSimulation or modeling
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

Citations9
Published2021
Admission routes1
Has abstractyes

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