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Record W2277706715 · doi:10.1002/cplu.201500558

Cysteine Radical/Metal Ion Adducts: A Gas‐Phase Structural Elucidation and Reactivity Study

2016· article· en· W2277706715 on OpenAlexafffund
Michael Lesslie, Justin Kai‐Chi Lau, John T. Lawler, K. W. Michael Siu, Vincent Steinmetz, Philippe Maı̂tre, Alan C. Hopkinson, Victor Ryzhov

Bibliographic record

VenueChemPlusChem · 2016
Typearticle
Languageen
FieldChemistry
TopicRadical Photochemical Reactions
Canadian institutionsUniversity of WindsorIONICS Mass Spectrometry (Canada)York University
FundersNatural Sciences and Engineering Research Council of CanadaShared Hierarchical Academic Research Computing NetworkNorthern Illinois University
KeywordsChemistryRadicalInfrared multiphoton dissociationAdductRadical ionDissociation (chemistry)PhotochemistryBond-dissociation energyAlkali metalDensity functional theoryReactivity (psychology)IonComputational chemistryPhysical chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Abstract The formation and investigation of sulfur‐based cysteine radicals cationized by a group 1A metal ion or Ag+ in the gas phase are reported. Gas‐phase ion–molecule reactions (IMR) and infrared multiple‐photon dissociation (IRMPD) spectroscopy revealed that the Li+, Na+, and K+ adducts of the cysteine radical remain S‐based radicals as initially formed. Theoretical calculations for the three alkali metal ions found that the lowest‐energy isomers are Cα‐based radicals, but they are not observed experimentally owing to the barriers associated with the hydrogen‐atom transfer. A mechanism for the S‐to‐Cα radical rearrangement in the metal ion complexes was proposed, and the relative energies of the associated energy barriers were found to be Li+>Na+>K+ at all levels of theory. Relative to the B3LYP functional, other levels of calculation gave significantly higher barriers (by 35–40 kJ mol−1 at MP2 and 44–47 kJ mol−1 at the CCSD level) using the same basis set. Unlike the alkali metal adducts, the cysteine radical/Ag+ complex rearranged from the S‐based radical to an unreactive species as indicated by IMRs and IRMPD spectroscopy. This is consistent with the Ag+/cysteine radical complex having a lower S‐to‐Cα radical conversion barrier, as predicted by the MP2 and CCSD levels of theory.

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 score0.005

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 studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
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 head0.016
GPT teacher head0.284
Teacher spread0.268 · 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

Citations10
Published2016
Admission routes2
Has abstractyes

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