Computational Investigation of a Series of Small Molecules as Potential Compounds for Lysyl Hydroxylase-2 (LH2) Inhibition

J Chem Inf Model. 2023 Feb 13;63(3):986-1001. doi: 10.1021/acs.jcim.2c01448. Epub 2023 Jan 30.

Abstract

The catalytic function of lysyl hydroxylase-2 (LH2), a member of the Fe(II)/αKG-dependent oxygenase superfamily, is to catalyze the hydroxylation of lysine to hydroxylysine in collagen, resulting in stable hydroxylysine aldehyde-derived collagen cross-links (HLCCs). Reports show that high amounts of LH2 lead to the accumulation of HLCCs, causing fibrosis and specific types of cancer metastasis. Some members of the Fe(II)/αKG-dependent family have also been reported to have intramolecular O2 tunnels, which aid in transporting one of the required cosubstrates into the active site. While LH2 can be a promising target to combat these diseases, efficacious inhibitors are still lacking. We have used computational simulations to investigate a series of 44 small molecules as lead compounds for LH2 inhibition. Tunneling analyses indicate the existence of several intramolecular tunnels. The lengths of the calculated O2-transporting tunnels in holoenzymes are relatively longer than those in the apoenzyme, suggesting that the ligands may affect the enzyme's structure and possibly block (at least partially) the tunnels. The sequence alignment analysis between LH enzymes from different organisms shows that all of the amino acid residues with the highest occurrence rate in the oxygen tunnels are conserved. Our results suggest that the enolate form of diketone compounds establishes stronger interactions with the Fe(II) in the active site. Branching the enolate compounds with functional groups such as phenyl and pyridinyl enhances the interaction with various residues around the active site. Our results provide information about possible leads for further LH2 inhibition design and development.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Collagen / chemistry
  • Collagen / metabolism
  • Ferrous Compounds
  • Hydroxylysine*
  • Lysine / metabolism
  • Procollagen-Lysine, 2-Oxoglutarate 5-Dioxygenase* / antagonists & inhibitors
  • Procollagen-Lysine, 2-Oxoglutarate 5-Dioxygenase* / chemistry

Substances

  • Collagen
  • Ferrous Compounds
  • Hydroxylysine
  • Lysine
  • Procollagen-Lysine, 2-Oxoglutarate 5-Dioxygenase