Structure, mechanism, and inhibition of Hedgehog acyltransferase

Mol Cell. 2021 Dec 16;81(24):5025-5038.e10. doi: 10.1016/j.molcel.2021.11.018. Epub 2021 Dec 9.

Abstract

The Sonic Hedgehog (SHH) morphogen pathway is fundamental for embryonic development and stem cell maintenance and is implicated in various cancers. A key step in signaling is transfer of a palmitate group to the SHH N terminus, catalyzed by the multi-pass transmembrane enzyme Hedgehog acyltransferase (HHAT). We present the high-resolution cryo-EM structure of HHAT bound to substrate analog palmityl-coenzyme A and a SHH-mimetic megabody, revealing a heme group bound to HHAT that is essential for HHAT function. A structure of HHAT bound to potent small-molecule inhibitor IMP-1575 revealed conformational changes in the active site that occlude substrate binding. Our multidisciplinary analysis provides a detailed view of the mechanism by which HHAT adapts the membrane environment to transfer an acyl chain across the endoplasmic reticulum membrane. This structure of a membrane-bound O-acyltransferase (MBOAT) superfamily member provides a blueprint for other protein-substrate MBOATs and a template for future drug discovery.

Keywords: Hedgehog acyl transferase; Sonic Hedgehog signaling; cryo-EM structure; drug; heme; integral membrane protein; membrane-bound O-acyltransferase; molecular dynamics simulations; palmitoyl co enzyme A; small molecule inhibitor.

Publication types

  • Research Support, Non-U.S. Gov't
  • Video-Audio Media

MeSH terms

  • Acylation
  • Acyltransferases / antagonists & inhibitors*
  • Acyltransferases / genetics
  • Acyltransferases / metabolism*
  • Acyltransferases / ultrastructure
  • Allosteric Regulation
  • Animals
  • COS Cells
  • Catalytic Domain
  • Chlorocebus aethiops
  • Cryoelectron Microscopy
  • Enzyme Inhibitors / pharmacology*
  • HEK293 Cells
  • Hedgehog Proteins / metabolism*
  • Heme / metabolism
  • Humans
  • Membrane Proteins / antagonists & inhibitors
  • Membrane Proteins / genetics
  • Membrane Proteins / metabolism*
  • Membrane Proteins / ultrastructure
  • Molecular Dynamics Simulation
  • Palmitoyl Coenzyme A / metabolism
  • Protein Conformation
  • Signal Transduction
  • Structure-Activity Relationship

Substances

  • Enzyme Inhibitors
  • Hedgehog Proteins
  • Membrane Proteins
  • SHH protein, human
  • Palmitoyl Coenzyme A
  • Heme
  • Acyltransferases
  • HHAT protein, human