Design of novel potent antihyperlipidemic agents with antioxidant/anti-inflammatory properties: exploiting phenothiazine's strong antioxidant activity

J Med Chem. 2014 Mar 27;57(6):2568-81. doi: 10.1021/jm401842e. Epub 2014 Mar 13.

Abstract

Because atherosclerosis is an inflammatory process involving a series of pathological events such as dyslipidemia, oxidative stress, and blood clotting mechanisms, we hereby report the synthesis and evaluation of novel compounds in which antioxidant, anti-inflammatory, and squalene synthase (SQS) inhibitory/hypolipidemic activities are combined in simple molecules through design. The coupling of two different pharmacophores afforded compounds 1-12, whose biological profile was markedly improved compared to those of parent lead structures (i.e., the hypolipidemic 2-hydroxy-2-aryl-(benzo)oxa(or thia)zine and the antioxidant phenothiazine). Most derivatives strongly inhibited in vitro microsomal lipid and LDL peroxidation, exhibiting potent free-radical scavenging activity. They further significantly inhibited SQS activity and showed remarkable antidyslipidemic activity in vivo in animal models of acute and high-fat-induced hyperlipidemia. Finally, several compounds showed anti-inflammatory activity in vitro, inhibiting cycloxygenase (COX-1/2) activity. The multimodal properties of the new compounds and especially their combined antioxidant/SQS/COX inhibitory activity render them interesting lead compounds for further evaluation against atherosclerosis.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Anti-Inflammatory Agents, Non-Steroidal / chemical synthesis*
  • Anti-Inflammatory Agents, Non-Steroidal / pharmacology*
  • Antioxidants / chemical synthesis*
  • Antioxidants / pharmacology*
  • Atherosclerosis / drug therapy
  • Biphenyl Compounds
  • Carrageenan
  • Cholesterol, Dietary / pharmacology
  • Cyclooxygenase Inhibitors / chemical synthesis
  • Cyclooxygenase Inhibitors / pharmacology
  • Diet, High-Fat
  • Drug Design
  • Edema / chemically induced
  • Edema / prevention & control
  • Enzyme Inhibitors / chemical synthesis
  • Enzyme Inhibitors / pharmacology
  • Farnesyl-Diphosphate Farnesyltransferase / antagonists & inhibitors
  • Hypolipidemic Agents / chemical synthesis*
  • Hypolipidemic Agents / pharmacology*
  • In Vitro Techniques
  • Indicators and Reagents
  • Lipid Peroxidation / drug effects
  • Magnetic Resonance Spectroscopy
  • Male
  • Mice
  • Microsomes / drug effects
  • Microsomes / metabolism
  • Phenothiazines / chemical synthesis*
  • Phenothiazines / pharmacology*
  • Picrates
  • Rats

Substances

  • Anti-Inflammatory Agents, Non-Steroidal
  • Antioxidants
  • Biphenyl Compounds
  • Cholesterol, Dietary
  • Cyclooxygenase Inhibitors
  • Enzyme Inhibitors
  • Hypolipidemic Agents
  • Indicators and Reagents
  • Phenothiazines
  • Picrates
  • Carrageenan
  • 1,1-diphenyl-2-picrylhydrazyl
  • Farnesyl-Diphosphate Farnesyltransferase