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Record W3203159251 · doi:10.26434/chemrxiv.12798083.v1

Online HPLC Analysis of Buchwald-Hartwig Aminations from Within an Inert Environment

2020· preprint· en· W3203159251 on OpenAlexafffund
Thomas C. Malig, Lars P. E. Yunker, Sebastian Steiner, Jason E. Hein

Bibliographic record

VenueChemRxiv · 2020
Typepreprint
Languageen
FieldChemistry
TopicCatalytic Cross-Coupling Reactions
Canadian institutionsUniversity of British Columbia
FundersNatural Sciences and Engineering Research Council of CanadaUniversity of British Columbia
KeywordsIodobenzeneChemistryCatalysisCombinatorial chemistryComputer scienceOrganic chemistry

Abstract

fetched live from OpenAlex

We have developed a reaction monitoring platform capable of automated sampling and online HPLC analysis to generate temporal profiles for reactions performed from within a glovebox. The device allows for facile reaction progress analysis to aid in mechanistic studies of air-sensitive chemical transformations. The platform has demonstrated high reproducibility regarding sample mixing, dilution, delivery, and analysis. We employed the sampling platform to acquire temporal profiles for a series of Buchwald-Hartwig aminations. Parallel coupling reactions using iodobenzene and bromobenzene both exhibit complex kinetics. A competition reaction including both aryl halides demonstrated high selectivity for iodobenzene indicative of catalyst monopoly. The temporal profile for the difunctionalized substrate 1,4-iodobromobenzene was unexpected based a priori and is indicative of a distinct underlying mechanism. We attribute this unanticipated reactivity to intramolecular catalysts transfer through the π system as seen in “living” polymerization transfer catalyst systems. This automated sampling platform has greatly increased mechanistic understanding by performing only a small subset of experiments.

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 score0.123
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.001
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0010.001
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 head0.036
GPT teacher head0.288
Teacher spread0.252 · 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

Citations0
Published2020
Admission routes2
Has abstractyes

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