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Record W1976280255 · doi:10.1021/cs401065n

Deracemization of 2-Methyl-1,2,3,4-Tetrahydroquinoline Using Mutant Cyclohexylamine Oxidase Obtained by Iterative Saturation Mutagenesis

2014· article· en· W1976280255 on OpenAlex
Guangyue Li, Jie Ren, Peiyuan Yao, Yitao Duan, Hailing Zhang, Qiaqing Wu, Jinhui Feng, Peter C. K. Lau, Dunming Zhu

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.

Bibliographic record

VenueACS Catalysis · 2014
Typearticle
Languageen
FieldBiochemistry, Genetics and Molecular Biology
TopicEnzyme Catalysis and Immobilization
Canadian institutionsMcGill UniversityNational Research Council CanadaCentre in Green Chemistry and Catalysis
Fundersnot available
KeywordsSaturated mutagenesisChemistryFlavin groupCyclohexylamineEnantiomeric excessMutagenesisStereoselectivitySubstrate (aquarium)Kinetic resolutionBiocatalysisAmine gas treatingStereochemistryMutantCombinatorial chemistryCatalysisOrganic chemistryBiochemistryEnantioselective synthesisReaction mechanismBiologyEnzymeGene

Abstract

fetched live from OpenAlex

The current toolkit of biocatalysts for the production of enantiomerically pure chiral amines is largely restricted to amine transaminases, ammonia lyases, or the genetic variants of monoamine oxidase N(MAO-N) from Aspergillus niger . Flavin-dependent amine oxidases have the apparent advantage of using molecular oxygen as a stoichiometric oxidant and their reactions are irreversible. To expand the toolkit and increase the substrate spectrum of a bacterial and flavin-dependent cyclohexylamine oxidase (CHAO) to enable deracemization of secondary amines, saturation mutagenesis of 11 amino acid residues located around the cyclohexanone substrate within a distance of 5 Å, followed by iterative saturation mutagenesis of four beneficial mutants, were performed. Screening with 2-methyl-1,2,3,4-tetrahydroquinoline as the substrate generated two improved CHAO variants, T198FL199S and T198FL199SM226F, that exhibited up to 406 times higher catalytic efficiency than the wild-type CHAO. Besides, high stereoselectivity for 2-methyl-1,2,3,4-tetrahydroquinoline and other 2-substituted-1,2,3,4-tetrahydroquinolines was demonstrated. In particular, deracemization of 2-methyl-1,2,3,4-tetrahydroquinoline by Escherichia coli whole cells expressing CHAO mutant T198FL199SM226F led to the production of ( R )-2-methyl-1,2,3,4-tetrahydroquinoline with high yield (76%) and enantiomeric excess (ee, 98%). Tetrahydroquinolines are important building blocks of natural and synthetic products useful in the pharmaceutical and agrochemical industries.

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.

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 score0.082
Threshold uncertainty score0.883

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.001
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 head0.006
GPT teacher head0.238
Teacher spread0.232 · 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