A Proteolytic Site-Directed Affinity Label to Inhibit the Human ATP-Dependent Protease Caseinolytic Complex XP.


Journal

Chembiochem : a European journal of chemical biology
ISSN: 1439-7633
Titre abrégé: Chembiochem
Pays: Germany
ID NLM: 100937360

Informations de publication

Date de publication:
16 07 2020
Historique:
received: 20 01 2020
revised: 01 03 2020
pubmed: 18 3 2020
medline: 23 6 2021
entrez: 18 3 2020
Statut: ppublish

Résumé

Human caseinolytic protease component X and P (hClpXP) is a heterooligomeric ATP-dependent protease. The hClpX subunit catalyzes ATP hydrolysis whereas the hClpP subunit catalyzes peptide bond cleavage. In this study, we generated a peptidyl chloromethyl ketone (dansyl-FAPAL-CMK) that inhibited the hClpP subunit through alkylation of the catalytic His122, which was detected by LC-MS. This inhibitor is composed of a peptide sequence derived from a hydrolyzed peptide product of a substrate cleaved by hClpXP. Binding of FAPAL positions the electrophilic chloromethyl ketone moiety near His122 where alkylation occurs. Dansyl FAPAL-CMK exhibits selectivity for hClpXP over other ATP-dependent proteases such as hLon and the 26S proteasome and abolishes hClpXP activity in HeLa cell lysate. Using the fluorogenic peptide substrate FR-Cleptide as reporter, we detected biphasic inhibition time courses; this supports a slow-binding, time-dependent, covalent inhibition mechanism that is often found in active-site directed affinity labels. Because this inhibitor reacts only with hClpXP but not hLon or the proteasome, it has the potential to serve as a chemical tool to help validate endogenous protein substrates of hClpXP in cell lysate, thereby benefiting investigation of the physiological functions of hClpXP in different cell types or tissue samples.

Identifiants

pubmed: 32180302
doi: 10.1002/cbic.202000031
doi:

Substances chimiques

Protease Inhibitors 0
Adenosine Triphosphate 8L70Q75FXE
ClpP protein, human EC 3.4.21.92
Endopeptidase Clp EC 3.4.21.92
CLPX protein, human EC 3.6.1.3

Types de publication

Journal Article Research Support, U.S. Gov't, Non-P.H.S.

Langues

eng

Sous-ensembles de citation

IM

Pagination

2049-2059

Informations de copyright

© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Auteurs

Zhou Sha (Z)

Department of Chemistry, Case Western Reserve University, Cleveland, Ohio, 44106, USA.

Sujatha Chilakala (S)

Department of Chemistry, Cleveland State University, Cleveland, Ohio, 44115, USA.
Present address: Lawrence J. Ellison Institute for Transformative Medicine of USC, University of Southern California, Beverly Hills, CA, 90211, USA.

George Crabill (G)

Department of Chemistry, Case Western Reserve University, Cleveland, Ohio, 44106, USA.
Present address: University of Maryland School of Medicine, Baltimore, MD, 21202, USA.

Iteen Cheng (I)

Department of Chemistry, Case Western Reserve University, Cleveland, Ohio, 44106, USA.
Present address: Agilent Technologies, Cleveland, OH, 44106, USA.

Yan Xu (Y)

Department of Chemistry, Cleveland State University, Cleveland, Ohio, 44115, USA.

Jennifer Fishovitz (J)

Department of Chemistry and Physics, Saint Mary's College, Notre Dame, Indiana, 46556, USA.

Irene Lee (I)

Department of Chemistry, Case Western Reserve University, Cleveland, Ohio, 44106, USA.

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