MétaCan
Menu
Back to cohort
Record W3127582876 · doi:10.1002/anie.202013920

Cysteine Nucleophiles in Glycosidase Catalysis: Application of a Covalent β‐<scp>l‐</scp>Arabinofuranosidase Inhibitor

2021· article· en· W3127582876 on OpenAlexfundno aff
Nicholas G. S. McGregor, Joan Coines, Valentina Borlandelli, Satoko Amaki, Marta Artola, Alba Nin‐Hill, Daniël Linzel, Chihaya Yamada, T. Arakawa, Akihiro Ishiwata, Yukishige Ito, Gijsbert A. van der Marel, Jeroen D. C. Codée, Shinya Fushinobu, Herman S. Overkleeft, Carme Rovira, G.J. Davies

Bibliographic record

VenueAngewandte Chemie International Edition · 2021
Typearticle
Languageen
FieldChemistry
TopicCarbohydrate Chemistry and Synthesis
Canadian institutionsnot available
FundersH2020 European Research CouncilAgencia Estatal de InvestigaciónBiotechnology and Biological Sciences Research CouncilNatural Sciences and Engineering Research Council of CanadaJapan Society for the Promotion of ScienceHorizon 2020 Framework ProgrammeBarcelona Supercomputing CenterDiamond Light SourceGeneralitat de CatalunyaMinisterio de Ciencia e InnovaciónNederlandse Organisatie voor Wetenschappelijk OnderzoekDirectorate for Biological SciencesAgència de Gestió d'Ajuts Universitaris i de RecercaRoyal SocietyMinisterio de Ciencia, Innovación y Universidades
KeywordsNucleophileChemistryCysteineCovalent bondStereochemistryAdductCatalysisThiolCombinatorial chemistryActive siteEnzymeOrganic chemistry

Abstract

fetched live from OpenAlex

(Glu) coordination complex, has presented unresolved mechanistic questions. In particular, the proposed mechanism, depending on a Zn-coordinated cysteine nucleophile and passing through a thioglycosyl enzyme intermediate, remains controversial. This is primarily due to the expected stability of the intermediate C-S bond. To facilitate the study of this atypical mechanism, we report the synthesis of a cyclophellitol-derived β-l-arabinofuranosidase inhibitor, hypothesised to react with the catalytic nucleophile to form a non-hydrolysable adduct analogous to the mechanistic covalent intermediate. This β-l-arabinofuranosidase inhibitor reacts exclusively with the proposed cysteine thiol catalytic nucleophiles of representatives of GH families 127 and 146. X-ray crystal structures determined for the resulting adducts enable MD and QM/MM simulations, which provide insight into the mechanism of thioglycosyl enzyme intermediate breakdown. Leveraging the unique chemistry of cyclophellitol derivatives, the structures and simulations presented here support the assignment of a zinc-coordinated cysteine as the catalytic nucleophile and illuminate the finely tuned energetics of this remarkable metalloenzyme clan.

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)0.001
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow)
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 score0.015
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.001
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 head0.009
GPT teacher head0.230
Teacher spread0.221 · 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

Citations25
Published2021
Admission routes1
Has abstractyes

Explore more

Same venueAngewandte Chemie International EditionSame topicCarbohydrate Chemistry and SynthesisFrench-language works237,207