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Record W4396580001 · doi:10.1002/celc.202400193

Overcoming Challenges in Electrosynthesis Using High‐Throughput Electrochemistry: Hypervalent Iodine‐Mediated Phenol Dearomatization, a Case Study

2024· article· en· W4396580001 on OpenAlexafffund
Antoine Juneau, Marzieh Abdolhosseini, Camille Rocq, Hanh D. M. Pham, Mia Pascall, Rustam Z. Khaliullin, Sylvain Canesi, Eric McCalla, Janine Mauzeroll

Bibliographic record

VenueChemElectroChem · 2024
Typearticle
Languageen
FieldChemistry
TopicOxidative Organic Chemistry Reactions
Canadian institutionsUniversité du Québec à MontréalMcGill University
FundersNatural Sciences and Engineering Research Council of CanadaCanada Foundation for Innovation
KeywordsElectrosynthesisHypervalent moleculeElectrochemistryCyclic voltammetryReproducibilityYield (engineering)RedoxPhenolSupporting electrolyteIodineElectrolyteChemistryRaman spectroscopyNanotechnologyCombinatorial chemistryMaterials scienceElectrodeInorganic chemistryOrganic chemistryPhysical chemistryChromatography

Abstract

fetched live from OpenAlex

Abstract Despite many recent efforts, the field of organic electrosyn‐thesis faces important challenges due to the intricate nature of heterogeneous redox processes, the wide parameter space to be explored and the lack of standardized methods. To overcome these limitations, we developed a cost‐effective high‐throughput electrochemical (HTE) reactor capable of running 24 individually controlled parallel reactions. This system allows the rapid testing of electrochemical parameters on a given reaction, assessing not only yield but also reproducibility. Using the hypervalent iodine‐mediated dearomatization of phloretic acid as a demonstration of HTE capabilities, we ran more than 200 electrosyntheses in different experimental conditions and demonstrate the effect of parameters such as total charge transferred, current, electrode materials, electrolyte formulation and concentration, mediator formulation and concentration and electrochemical technique of oxidation. Notably, this report demonstrates that while catalytic amounts of iodine mediator can be used successfully, the reproducibility may be affected, which calls for a cautious approach when developing similar transformations. Using cyclic voltammetry, density functional theory, chronopotentiometry, and Raman spectroscopy, we shed light on the causes of this issue.

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)0.002
metaresearch head score (Gemma)0.001
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 score0.011

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0020.001
Meta-epidemiology (narrow)0.0010.000
Meta-epidemiology (broad)0.0000.001
Bibliometrics0.0010.001
Science and technology studies0.0010.001
Scholarly communication0.0020.002
Open science0.0010.001
Research integrity0.0010.002
Insufficient payload (model declined to judge)0.0010.001

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 head0.044
GPT teacher head0.282
Teacher spread0.238 · 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

Citations7
Published2024
Admission routes2
Has abstractyes

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