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A programmable chemical switch based on triggerable Michael acceptors

Jiaming Zhuang, Bo Zhao, Xiangxi Meng, Jessica D. Schiffman, Sarah L. Perry, Richard W. Vachet, S. Thayumanavan

2020Chemical Science58 citationsDOIOpen Access PDF

Abstract

, thiols and amines. This thiol/amine-triggerable chemical switch is based on a Triggerable Michael Acceptor (TMAc) which bears good leaving groups at its β-position. The acceptor undergoes a "trigger-to-release" process where thiol/amine addition triggers cascaded release of leaving groups and generates a less activated acceptor. The newly generated TMAc can be further reversed to liberate the original thiol/amine by a second nucleophile trigger through a "trigger-to-reverse" process. Within the small molecular volume of the switch, we have shown five locations that can be engineered to achieve tunable "trigger-to-release" kinetics and tailored reversibility. The potential of the engineerable bonding/debonding capability of the chemical switch is demonstrated by applications in cysteine-selective and reversible protein modification, universal self-immolative linkers, and orthogonally addressable hydrogels.

Topics & Concepts

LinkerDecoupling (probability)Michael reactionAcceptorCombinatorial chemistryChemistryNanotechnologyMaterials scienceOrganic chemistryComputer scienceEngineeringPhysicsCatalysisCondensed matter physicsControl engineeringOperating systemClick Chemistry and ApplicationsChemical Synthesis and AnalysisMolecular Junctions and Nanostructures
A programmable chemical switch based on triggerable Michael acceptors | Litcius