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Record W4307730773 · doi:10.1002/qua.27024

New insights into phosphorus biphilicity: Stereochemistry of monocyclic aminophosphoranes formation

2022· article· en· W4307730773 on OpenAlex
Alia Méjri, Outaf Fliss, K. Essalah, Mohamed Ali Boughdiri, Fabien Picaud, Bahoueddine Tangour, Abdelhamid Sayari

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

VenueInternational Journal of Quantum Chemistry · 2022
Typearticle
Languageen
FieldChemistry
TopicOrganophosphorus compounds synthesis
Canadian institutionsUniversity of Ottawa
FundersNatural Sciences and Engineering Research Council of Canada
KeywordsChemistryPhosphoraneNucleophileTransition stateElectrophileReactivity (psychology)Reaction coordinateComputational chemistryStereochemistryYlideAmine gas treatingReaction mechanismMedicinal chemistryCatalysisOrganic chemistry

Abstract

fetched live from OpenAlex

Abstract Oxidative addition of aliphatic amine on monocyclic 2‐R‐1,3,2‐dioxaphospholane (R = methyl or phenyl) leading to phosphoranes bearing a PH axial bond was investigated using a combined theoretical and experimental approach. The reaction followed first order kinetics for both reactants. The activation parameters were consistent with a concerted mechanism exhibiting stereo, enantio, and regio specificities. Systematic density functional theory studies including reactivity descriptors, structural parameters, determination of all possible phosphorane isomers, their transition states and their formation mechanisms were carried out to delineate the reaction pathway. Depending on the nature of the atom in the final apical position (H, N of the amine, or C of the methyl), three types of phosphoranes were identified. Energy profiles, using the intrinsic reaction coordinate technique for the formation of each isomer, were established. It was shown that the phosphorus biphilicity acts in three consecutive sequences, namely nitrogen nucleophilic attack leading to a supermolecule structure, nucleophilic behavior of phosphorus in the transition state zone of influence, and electrophilic approach of the nitrogen atom to complete the reaction. Phosphorane with an equatorial PH bond was found to be a kinetic product that transforms rapidly to the thermodynamically stable isomer with axial PH via two consecutive Berry pseudo‐rotations. A new tool, referred to reactive internal reaction coordinates, was introduced to represent the reaction path more clearly.

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), 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 score0.018
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0020.001
Research integrity0.0000.001
Insufficient payload (model declined to judge)0.0040.000

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 head0.011
GPT teacher head0.235
Teacher spread0.224 · 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