Using sulfuramidimidoyl fluorides that undergo sulfur(VI) fluoride exchange for inverse drug discovery.


Journal

Nature chemistry
ISSN: 1755-4349
Titre abrégé: Nat Chem
Pays: England
ID NLM: 101499734

Informations de publication

Date de publication:
10 2020
Historique:
received: 25 04 2019
accepted: 23 07 2020
pubmed: 2 9 2020
medline: 23 2 2021
entrez: 2 9 2020
Statut: ppublish

Résumé

Drug candidates that form covalent linkages with their target proteins have been underexplored compared with the conventional counterparts that modulate biological function by reversibly binding to proteins, in part due to concerns about off-target reactivity. However, toxicity linked to off-target reactivity can be minimized by using latent electrophiles that only become activated towards covalent bond formation on binding a specific protein. Here we study sulfuramidimidoyl fluorides, a class of weak electrophiles that undergo sulfur(VI) fluoride exchange chemistry. We show that equilibrium binding of a sulfuramidimidoyl fluoride to a protein can allow nucleophilic attack by a specific amino acid side chain, which leads to conjugate formation. We incubated small molecules, each bearing a sulfuramidimidoyl fluoride electrophile, with human cell lysate, and the protein conjugates formed were identified by affinity chromatography-mass spectrometry. This inverse drug discovery approach identified a compound that covalently binds to and irreversibly inhibits the activity of poly(ADP-ribose) polymerase 1, an important anticancer target in living cells.

Identifiants

pubmed: 32868886
doi: 10.1038/s41557-020-0530-4
pii: 10.1038/s41557-020-0530-4
pmc: PMC7541551
mid: NIHMS1614419
doi:

Substances chimiques

Sulfhydryl Compounds 0
Sulfur 70FD1KFU70
Fluorides Q80VPU408O

Types de publication

Journal Article Research Support, N.I.H., Extramural Research Support, Non-U.S. Gov't

Langues

eng

Sous-ensembles de citation

IM

Pagination

906-913

Subventions

Organisme : NIEHS NIH HHS
ID : P42 ES004699
Pays : United States
Organisme : NIDDK NIH HHS
ID : R01 DK046335
Pays : United States
Organisme : NIEHS NIH HHS
ID : R01 ES002710
Pays : United States
Organisme : NIDDK NIH HHS
ID : R37 DK046335
Pays : United States
Organisme : NIEHS NIH HHS
ID : R35 ES030443
Pays : United States

Commentaires et corrections

Type : CommentIn
Type : CommentIn

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Auteurs

Gabriel J Brighty (GJ)

Department of Chemistry, The Scripps Research Institute, La Jolla, CA, USA.
Department of Molecular Medicine, The Scripps Research Institute, La Jolla, CA, USA.

Rachel C Botham (RC)

Department of Chemistry, The Scripps Research Institute, La Jolla, CA, USA.
Department of Molecular Medicine, The Scripps Research Institute, La Jolla, CA, USA.
Codexis, Redwood City, CA, USA.

Suhua Li (S)

Department of Chemistry, The Scripps Research Institute, La Jolla, CA, USA.
School of Chemistry, Sun Yat-Sen University, Guangzhou, P. R. China.

Luke Nelson (L)

Department of Chemistry, The Scripps Research Institute, La Jolla, CA, USA.

David E Mortenson (DE)

Department of Chemistry, The Scripps Research Institute, La Jolla, CA, USA.
Department of Molecular Medicine, The Scripps Research Institute, La Jolla, CA, USA.
Gilead Sciences Inc., Foster City, CA, USA.

Gencheng Li (G)

Department of Chemistry, The Scripps Research Institute, La Jolla, CA, USA.

Christophe Morisseau (C)

Department of Entomology and Nematology, University of California Davis, Davis, CA, USA.
UC Davis Comprehensive Cancer Center, University of California Davis, Davis, CA, USA.

Hua Wang (H)

Department of Chemistry, The Scripps Research Institute, La Jolla, CA, USA.
Sorrento Therapeutics, Inc., San Diego, CA, USA.

Bruce D Hammock (BD)

Department of Entomology and Nematology, University of California Davis, Davis, CA, USA.
UC Davis Comprehensive Cancer Center, University of California Davis, Davis, CA, USA.

K Barry Sharpless (KB)

Department of Chemistry, The Scripps Research Institute, La Jolla, CA, USA. sharples@scripps.edu.
The Skaggs Institute for Chemical Biology, The Scripps Research Institute, La Jolla, CA, USA. sharples@scripps.edu.

Jeffery W Kelly (JW)

Department of Chemistry, The Scripps Research Institute, La Jolla, CA, USA. jkelly@scripps.edu.
Department of Molecular Medicine, The Scripps Research Institute, La Jolla, CA, USA. jkelly@scripps.edu.
The Skaggs Institute for Chemical Biology, The Scripps Research Institute, La Jolla, CA, USA. jkelly@scripps.edu.

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