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Record W7117368346 · doi:10.1002/ange.202522762

A Biocatalytic Platform for the Synthesis of Organofunctional Silanes and Siloxanes

2025· article· en· W7117368346 on OpenAlexaff
Tyler J. Fulton, Ryan R. Maar, John M. Roberts, Dimitris E. Katsoulis, Frances H. Arnold

Bibliographic record

VenueAngewandte Chemie · 2025
Typearticle
Languageen
FieldChemistry
TopicCyclopropane Reaction Mechanisms
Canadian institutionsDow Chemical (Canada)
Fundersnot available
KeywordsSilanesCyclopropanationEnantioselective synthesisCarbeneDiazoBiocatalysis

Abstract

fetched live from OpenAlex

Abstract Organofunctional silanes are highly useful reagents in material science, functioning as effective crosslinking agents and adhesion promoters. Traditionally, their synthesis relies on precious transition‐metal catalysts, which require downstream purification and increase overall costs. Herein, we present a green and sustainable biocatalytic platform for the enantioselective synthesis of diverse organofunctional silanes bearing ester and cyano groups. Directed evolution of Thermus amyloliquefaciens protoglobin ( Tam Pgb) produced efficient enzymes for cyclopropanation of vinyl silanes and siloxanes using diazo compounds and N ‐tosylhydrazones as carbene precursors with excellent diastereo‐ and enantiocontrol (up to 2500 TTN, >99% dr, >99% ee). Notably, we demonstrate for the first time that N ‐tosylhydrazones can serve as carbene precursors in enzymatic reactions, providing a safer and more practical alternative for industrial applications.

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 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 score0.037
Threshold uncertainty score0.339

Codex and Gemma teacher scores by category

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)0.0000.000

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 head0.015
GPT teacher head0.237
Teacher spread0.222 · 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.

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

Citations0
Published2025
Admission routes1
Has abstractyes

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