Total Chemical Synthesis of a Nonfibrillating Human Glycoinsulin

J Am Chem Soc. 2020 Jan 22;142(3):1164-1169. doi: 10.1021/jacs.9b11424. Epub 2020 Jan 9.

Abstract

Glycosylation is an accepted strategy to improve the therapeutic value of peptide and protein drugs. Insulin and its analogues are life-saving drugs for all type I and 30% of type II diabetic patients. However, they can readily form fibrils which is a significant problem especially for their use in insulin pumps. Because of the solubilizing and hydration effects of sugars, it was thought that glycosylation of insulin could inhibit fibril formation and lead to a more stable formulation. Since enzymatic glycosylation results in heterogeneous products, we developed a novel chemical strategy to produce a homogeneous glycoinsulin (disialo-glycoinsulin) in excellent yield (∼60%). It showed a near-native binding affinity for insulin receptors A and B in vitro and high glucose-lowering effects in vivo, irrespective of the route of administration (s.c. vs i.p.). The glycoinsulin retained insulin-like helical structure and exhibited improved stability in human serum. Importantly, our disialo-glycoinsulin analogue does not form fibrils at both high concentration and temperature. Therefore, it is an excellent candidate for clinical use in insulin pumps.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Glucose / chemistry*
  • Glycosylation
  • Humans
  • Insulin / chemical synthesis*
  • Insulin / chemistry
  • Microscopy, Atomic Force

Substances

  • Insulin
  • Glucose