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Record W2032750615 · doi:10.1021/jp040513i

An Ab Initio and Density Functional Theory Study of Keto−Enol Equilibria of Hydroxycyclopropenone in Gas and Aqueous Solution Phase

2005· article· en· W2032750615 on OpenAlexaff
Stuart W. Paine, A. J. Kresge, A. Salam

Bibliographic record

VenueThe Journal of Physical Chemistry A · 2005
Typearticle
Languageen
FieldChemistry
TopicSynthesis and Biological Evaluation
Canadian institutionsUniversity of Toronto
Fundersnot available
KeywordsTautomerPolarizable continuum modelChemistryBasis setDensity functional theoryAb initioEnolGibbs free energyAqueous solutionComputational chemistryThermodynamicsPhysical chemistrySolvent effectsSolventOrganic chemistryPhysicsCatalysis

Abstract

fetched live from OpenAlex

Keto-enol tautomerism in hydroxycyclopropenone (2-hydroxy-2-cyclopropen-1-one) has been studied using ab initio methods, the B3LYP functional of density functional theory, as well as complete basis set (CBS-QB3 and CBS-APNO) and G3 methods. Absolute and relative energies were calculated with each of the methods, whereas computations of geometries and harmonic frequencies for hydroxycyclopropenone and 1,2-cyclopropanedione were computed in the gas phase but were limited to HF, MP2 and CCSD levels of theory, and the B3LYP functional, in combination with the 6-31++G** basis set. Using the MP2/6-31++G** gas phase optimized structure, each species was then optimized fully in aqueous solution by employing the polarizable continuum model (PCM) self-consistent reaction field approach, in which HF, MP2 and B3LYP levels of theory were utilized, with the same 6-31++G** basis set. In both gas and aqueous solution phases, the keto form is higher in energy for all of the model chemistries considered. The presence of the solvent, however, is found to have very little effect on the bond lengths, angles and harmonic frequencies. From the B3LYP/6-31++G** Gibbs free energy, the keto-enol tautomeric equilibrium constant for 2-hydroxy-2-cyclopropen-1-one <==> 1,2-cyclopropanedione is computed to be K(T)(gas) = 2.35 x 10(-6), K(T)(aq) = 5.61 x 10(-14). It is concluded that the enol form is overwhelmingly predominant in both environments, with the effect of the solvent shifting the direction of equilibrium even more strongly in the favor of hydroxycyclopropenone. The almost exclusive nature of this species is attributed to stabilization resulting from aromaticity. Confirmation is provided by comparison of the simulated vibrational spectra of hydroxycyclopropenone with the measured infrared spectrum in an argon matrix.

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: none
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.003
Threshold uncertainty score0.007

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0010.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0010.001
Insufficient payload (model declined to judge)0.0020.000

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 head0.030
GPT teacher head0.292
Teacher spread0.262 · 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

Citations20
Published2005
Admission routes1
Has abstractyes

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