Interactive Bioconjugation at N-Terminal Cysteines by Using O-Salicylaldehyde Esters towards Dual Site-Selective Functionalization

Chemistry. 2022 Dec 1;28(67):e202202377. doi: 10.1002/chem.202202377. Epub 2022 Nov 14.

Abstract

N-terminal Cys modification has been intensively studied to produce homogeneous bioconjugates essentially through two modes of reaction: reversible modification with the equilibrium shifted towards the formation of the desired conjugate or stable and irreversible conjugates. Herein, we report a new method of N-terminal cysteine modification using O-salicylaldehyde esters (OSAEs) through fast conjugation and irreversible deconjugation. These reagents can rapidly react with N-terminal Cys at low-micromolar concentration to form thiazolidines with subsequent hydrolysis of the ester moiety to the phenolic derivative. These phenolic thiazolidines can be hydrolyzed at acidic pH (≈4.5) to recover the intact N-terminal Cys. Bioconjugation reactions using OSAEs offer controlled reversibility to as act as a protecting group for N-terminal cysteines, allowing the modification of in-chain residues without perturbing the N-terminal Cys, which can then be deprotected and used as a conjugation site.

Keywords: N-terminal cysteine; bioconjugation; irreversible deconjugation; protecting group.

MeSH terms

  • Aldehydes*
  • Cysteine* / chemistry
  • Esters / chemistry
  • Thiazolidines

Substances

  • Cysteine
  • salicylaldehyde
  • Thiazolidines
  • Aldehydes
  • Esters