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Record W2072357435 · doi:10.1021/om800761c

Probing the Dynamics and Reactivity of a Stereochemically Nonrigid Cp*Ru(H)(κ<sup>2</sup>-<i>P</i>,<i>C</i>arbene) Complex

2008· article· en· W2072357435 on OpenAlexafffund
M.A. Rankin, D.F. MacLean, Robert McDonald, Michael J. Ferguson, Michael D. Lumsden, Mark Stradiotto

Bibliographic record

VenueOrganometallics · 2008
Typearticle
Languageen
FieldChemistry
TopicOrganoboron and organosilicon chemistry
Canadian institutionsUniversity of AlbertaDalhousie University
FundersNatural Sciences and Engineering Research Council of CanadaMcMaster University
KeywordsChemistryHydrideAdductReactivity (psychology)IndeneBoraneMedicinal chemistryReaction rate constantStereochemistryRutheniumNuclear magnetic resonance spectroscopyCrystallographyHydrogenKineticsOrganic chemistryCatalysis

Abstract

fetched live from OpenAlex

The ability of the coordinatively saturated, 18-electron Cp*(H)Ru═CHR complex 1 to serve as a masked source of the coordinatively unsaturated Cp*Ru-CH 2 R species 2 via reversible α-hydride elimination was surveyed. The rate constant for this dynamic process (300 K, C 6 D 6 ) was measured to be 59 ± 1 s −1, on the basis of data obtained from selective inversion NMR experiments. Exposure of 1 to an atmosphere of CO or to an equivalent of either PMe 3 or PH 2 Ph afforded the corresponding 2·L adduct (L = CO, 98%; PMe 3, 93%; PH 2 Ph, 67%). Treatment of 1 with Ph 2 SiH 2, PhSiH 3, Ph 2 SiClH, or PhSiClH 2 afforded the corresponding net Si−H addition product, 3a − d (82−94%); an NMR spectroscopic investigation of the analogous reaction of 1 with Ph 2 SiD 2 provided evidence in support of a reaction mechanism involving previously undocumented Si−H addition across the Ru═C unit in 1 in the formation of 3a . Addition of Jutzi’s acid (H(OEt 2 ) 2 B(C 6 F 5 ) 4 ) to 1 resulted in the quantitative formation of 4 (the N- C - H cyclometalated variant of [Cp*Ru(κ 2 -2- N Me 2 -3- P i Pr 2 -indene)] + B(C 6 F 5 ) 4 − ). In monitoring the progress of the reaction of 1 with excess catecholborane (HBcat), evidence for the formation of the B−H addition product 5i was obtained en route to the isolable (Bcat)Ru═C species ( 5, 54%). Conversely, no intermediates were observed in the reaction of 1 with mesitylborane (MesBH 2 ) leading to the Cp*Ru(P,N) complex 6 (81%), which features a tethered borane fragment and a Ru−H−B bridge. Crystallographic characterization data are provided for 2·PMe 3, 3a, 3b, 3d, 5, and 6 .

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)0.000
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 score0.009
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 studies0.0000.001
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 head0.019
GPT teacher head0.220
Teacher spread0.202 · 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

Citations36
Published2008
Admission routes2
Has abstractyes

Explore more

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