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Structure-based design of a phosphotyrosine-masked covalent ligand targeting the E3 ligase SOCS2

2023· preprint· en· W4385875205 on OpenAlexfundno aff
Sarath Ramachandran, Nikolai Makukhin, Kevin Haubrich, Manjula Nagala, Beth Forrester, Dylan M. Lynch, Ryan Casement, Andrea Testa, Elvira Bruno, Rosaria Gitto, Alessio Ciulli

Bibliographic record

VenueChemRxiv · 2023
Typepreprint
Languageen
FieldMedicine
TopicPeptidase Inhibition and Analysis
Canadian institutionsnot available
FundersEuropean Research CouncilMedical Research CouncilInnovative Medicines InitiativeUniversity of TorontoWellcome TrustEuropean Synchrotron Radiation FacilityEuropean CommissionDiamond Light Source
KeywordsCovalent bondChemistryUbiquitin ligaseDNA ligaseBiochemistrySH2 domainStereochemistryUbiquitinProto-oncogene tyrosine-protein kinase SrcSignal transductionEnzyme

Abstract

fetched live from OpenAlex

The Src homology 2 (SH2) domain recognises phosphotyrosine (pY) post translational modifications in partner proteins to trigger downstream signalling. Drug discovery efforts targeting the SH2 domains have long been stymied by the poor drug-like properties of phosphate and its mimetics. Here, we have used structure-based design to target the SH2 domain of the E3 ligase suppressor of cytokine signalling 2 (SOCS2). Starting from the highly ligand-efficient pY amino acid, a fragment growing approach led to a serendipitous observation of covalent modification of Cys111 in a co-crystal structure, which we leveraged to rationally design a cysteine-directed electrophilic covalent inhibitor MN551. We developed the prodrug MN714 containing a pivaloyloxymethyl (POM) protecting group and evidence its cell permeability and capping group unmasking using cellular target engagement and in cell 19F NMR spectroscopy. Covalent engagement and modification of Cys111 of cellular SOCS2 was confirmed using mass spectrometry. The qualified covalent inhibitors of SOCS2 could find attractive applications as chemical probes to understand the biology of SOCS2 and its CRL5 complex, and as covalent E3 ligase handles in proteolysis targeting chimera (PROTACs) to induce targeted protein degradation.

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)0.001
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 score0.022
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.001
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 head0.044
GPT teacher head0.286
Teacher spread0.242 · 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

Citations1
Published2023
Admission routes1
Has abstractyes

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