Site selective C-H functionalization of Mitragyna alkaloids reveals a molecular switch for tuning opioid receptor signaling efficacy

Nat Commun. 2021 Jun 22;12(1):3858. doi: 10.1038/s41467-021-23736-2.

Abstract

Mitragynine (MG) is the most abundant alkaloid component of the psychoactive plant material "kratom", which according to numerous anecdotal reports shows efficacy in self-medication for pain syndromes, depression, anxiety, and substance use disorders. We have developed a synthetic method for selective functionalization of the unexplored C11 position of the MG scaffold (C6 position in indole numbering) via the use of an indole-ethylene glycol adduct and subsequent iridium-catalyzed borylation. Through this work we discover that C11 represents a key locant for fine-tuning opioid receptor signaling efficacy. 7-Hydroxymitragynine (7OH), the parent compound with low efficacy on par with buprenorphine, is transformed to an even lower efficacy agonist by introducing a fluorine substituent in this position (11-F-7OH), as demonstrated in vitro at both mouse and human mu opioid receptors (mMOR/hMOR) and in vivo in mouse analgesia tests. Low efficacy opioid agonists are of high interest as candidates for generating safer opioid medications with mitigated adverse effects.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Analgesics / chemistry
  • Analgesics / pharmacology
  • Animals
  • Ethylene Glycol / chemistry
  • Humans
  • Mice
  • Mice, Knockout
  • Mitragyna / chemistry*
  • Models, Chemical
  • Molecular Structure
  • Plant Extracts / chemistry
  • Plant Extracts / pharmacology*
  • Protein Binding
  • Receptors, Opioid, mu / agonists*
  • Receptors, Opioid, mu / genetics
  • Receptors, Opioid, mu / metabolism
  • Secologanin Tryptamine Alkaloids / chemistry
  • Secologanin Tryptamine Alkaloids / pharmacology*

Substances

  • Analgesics
  • Plant Extracts
  • Receptors, Opioid, mu
  • Secologanin Tryptamine Alkaloids
  • 7-hydroxymitragynine
  • Ethylene Glycol