Regulating the Master Regulator: Controlling Ubiquitination by Thinking Outside the Active Site

J Med Chem. 2018 Jan 25;61(2):405-421. doi: 10.1021/acs.jmedchem.6b01346. Epub 2017 Feb 28.

Abstract

The labeling of proteins with ubiquitin/ubiquitin-like (Ubl) proteins is crucial for several physiological processes and in the onset of various diseases. Recently, targeting ubiquitin protein labeling has shifted toward the use of allosteric mechanisms over classical activity-based approaches. Allosteric enzyme regulation offers the potential for greater selectivity and has demonstrated less susceptibility to acquired resistance often associated with active site inhibitors. Furthermore, the isoform diversity among E1 activating, E2 conjugating, E3 ligase, and deubiquitinating (DUB) enzymes offers an ideal platform for modulating activity via allostery. Herein, we have reviewed allosteric inhibitors of the ubiquitin E1-E2-E3 and DUB enzymatic cascade developed over the past decade with a focus on their mechanisms of action. We have highlighted the advantages as well as the challenges associated with designing allosteric modulators of the ubiquitin labeling machinery, and the future promise in targeting these systems using allosteric approaches.

Publication types

  • Research Support, Non-U.S. Gov't
  • Review

MeSH terms

  • Allosteric Regulation
  • Catalytic Domain
  • Deubiquitinating Enzymes / antagonists & inhibitors*
  • Deubiquitinating Enzymes / chemistry
  • Deubiquitinating Enzymes / metabolism
  • Enzyme Inhibitors / chemistry*
  • Enzyme Inhibitors / pharmacology*
  • Humans
  • Protein Processing, Post-Translational
  • Thalidomide / pharmacology
  • Ubiquitin / metabolism
  • Ubiquitin-Activating Enzymes / antagonists & inhibitors*
  • Ubiquitin-Activating Enzymes / chemistry
  • Ubiquitin-Activating Enzymes / metabolism
  • Ubiquitin-Conjugating Enzymes / antagonists & inhibitors*
  • Ubiquitin-Conjugating Enzymes / chemistry
  • Ubiquitin-Conjugating Enzymes / metabolism
  • Ubiquitin-Protein Ligases / antagonists & inhibitors
  • Ubiquitination

Substances

  • Enzyme Inhibitors
  • Ubiquitin
  • Thalidomide
  • Ubiquitin-Conjugating Enzymes
  • Ubiquitin-Protein Ligases
  • Deubiquitinating Enzymes
  • Ubiquitin-Activating Enzymes