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Record W2052996559 · doi:10.1021/jo010379n

The Historic Camphenyl Cation:  A Detailed Structure Evaluation Including Solvation Energy Calculations

2001· article· en· W2052996559 on OpenAlexaff
Patrick Brunelle, Ted S. Sorensen, Christoph Taeschler

Bibliographic record

VenueThe Journal of Organic Chemistry · 2001
Typearticle
Languageen
FieldChemistry
TopicFree Radicals and Antioxidants
Canadian institutionsUniversity of Calgary
Fundersnot available
KeywordsCarbocationChemistrySolvationComputational chemistryPotential energy surfaceMaxima and minimaIonChemical physicsMoleculeOrganic chemistry

Abstract

fetched live from OpenAlex

The structure of the camphenyl cation 1 has been studied in detail, using both experimental and computational approaches. Like others, we find only one structure on the camphenyl-isobornyl cation PE surface, but this single structure shows some unusual features. These include a very soft PE surface for movement along the C2-C6 axis (a nonbonding distance in a classical description of the cation), and a result of this is that very high computational methods (optimization at MP4 or QCI levels) are required in order to get structural minima that "fit" the experimental data. This PE surface has been probed computationally using fixed C2-C6 distances, and when one also calculates chemical shifts for these "fixed" structures, one sees calculated (13)C NMR chemical shifts for the C2 carbon that are hugely dependent on this fixed distance value, giving near-linear slopes of ca. 25 ppm/0.1 A distance change. Since this distance can vary over at least 0.6 A with relatively small calculated energy changes, there is a total range of ca. 150 ppm involved here. In a second part of this work, and in response to a recent paper in which the historic Meerwein "carbocation intermediate" proposal was rejected, we have calculated solvation energies (SCI-PCM method) for four carbocation systems, including 1. We find carbocation solvation energies (epsilon = 10 "solvent") of 45-53 kcal/mol, and where comparison can be made, the data correlate well with the literature. On the basis of these results, we re-affirm the Meerwein "carbocation" mechanism, but in order to accommodate only a single carbocation intermediate, we offer a description that amounts to a subtle variation of both the nonclassical ion proposal and Meerwein's "two cation" mechanism, namely that the camphenyl cation, 1, as a ground-state structure, can be described as only very weakly interacting in the C2-C6 bridging sense, but that the PE surface along this "bond" is so shallow that an energy input of only 4-6 kcal/mol can produce a bridged "structure". This mechanism explains the preferred formation of exo products in both the camphenyl and isobornyl systems, isotopic exchange of chloride in camphenyl chloride, and it allows for partial racemization of the camphenyl-isobornyl products in the reaction.

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)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesInsufficient 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 score0.071
Threshold uncertainty score0.998

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
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 integrity0.0000.000
Insufficient payload (model declined to judge)0.0030.000

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 head0.019
GPT teacher head0.251
Teacher spread0.231 · 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

Citations16
Published2001
Admission routes1
Has abstractyes

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