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Record W2757205258 · doi:10.1021/acs.jpcb.7b07586

Interconversion between 4-Imidazolone Ions; Isomers of [b<sub>4</sub>]<sup>+</sup> Derived from Protonated Tetraglycine

2017· article· en· W2757205258 on OpenAlexafffund
K. H. Brian Lam, Justin Kai‐Chi Lau, Cheuk‐Kuen Lai, Alan C. Hopkinson, K. W. Michael Siu

Bibliographic record

VenueThe Journal of Physical Chemistry B · 2017
Typearticle
Languageen
FieldChemistry
TopicMass Spectrometry Techniques and Applications
Canadian institutionsUniversity of WindsorYork University
FundersNatural Sciences and Engineering Research Council of Canada
KeywordsChemistryProtonationIonDissociation (chemistry)MoleculeDeuteriumCrystallographyAmideIminePolyatomic ionStereochemistryPhysical chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Collision-induced dissociations of isotopically labeled protonated tetraglycines establish that the [b 4 ] + ion formed by loss of water from the second amide bond (structure II ) rearranges to form N 1 -protonated 3,5-dihydro-4 H -imidazol-4-one (structure I ), the product of water loss from the first amide bond. Structure II is slightly higher in energy than I (Δ H at 0 K is 5.1 kJ mol –1, as calculated at M06-2X/6-311++G-(d,p)), and the barrier to interconversion is 139.8 kJ mol –1 above I . The dominant dissociation pathway is the loss of methanimine (HN=CH 2 ) from ion I with a barrier of 167.1 kJ mol –1, giving [GlyGlyGlyGly + H – H 2 O – HN=CH 2 ] +, ion III; a minor channel, loss of NH 3, has a slightly higher barrier (181.5 kJ mol –1 ). Using labeled glycine ( 13 C α ) it was determined that loss of the imine is from the same residue as that from which water was initially lost. The collision-induced dissociation spectra of ion III derived from both I and II were identical, and their energy-resolved curves were also very similar. Ion III fragments by losses of a glycine molecule (the dominant channel), a water molecule, and a glycine residue (57 Da), giving ions IV, V, and VII, respectively. Isotopic labeling established the origins of each of the neutral molecules that are lost. Using glycine (2,2 D 2 ), rapid deuterium exchange was observed for both ions I and II for the α-hydrogens that are from the same residue as that from which the water had been eliminated.

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: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.002
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 studies0.0000.001
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.001
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 head0.014
GPT teacher head0.259
Teacher spread0.246 · 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 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

Citations6
Published2017
Admission routes2
Has abstractyes

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