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Multi-Stimuli-Responsive Amphiphilic Assemblies through Simple Postpolymerization Modifications.

ABSTRACT: A strategy to construct different stimuli responsive polymers from post polymerization modifications of a single polymer scaffold via thiol-disulfide exchange has been developed. Here, we report on a random copolymer that enables the design and syntheses of a series of dual or multi-stimuli responsive nanoassemblies using a simple post-polymerization modification step. The reactive functional group involves a side chain monopyridyl disulfide unit, which rapidly and quantitatively reacts with various thiols under mild conditions. Independent and concurrent incorporation of physical, chemical or biologically responsive properties have been demonstrated. We envision that this strategy may open up opportunities to simplify the synthesis of multi-functional polymers with broad implications in a variety of biological applications.

SUBMITTER: Liu X

PROVIDER: S-EPMC5774634 | biostudies-literature | 2016 Sep

REPOSITORIES: biostudies-literature

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Multi-Stimuli-Responsive Amphiphilic Assemblies through Simple Postpolymerization Modifications.

Liu Xiaochi X Hu Ding D Jiang Ziwen Z Zhuang Jiaming J Xu Yisheng Y Guo Xuhong X Thayumanavan S S

Macromolecules 20160816 17

A strategy to construct different stimuli responsive polymers from post polymerization modifications of a single polymer scaffold via thiol-disulfide exchange has been developed. Here, we report on a random copolymer that enables the design and syntheses of a series of dual or multi-stimuli responsive nanoassemblies using a simple post-polymerization modification step. The reactive functional group involves a side chain monopyridyl disulfide unit, which rapidly and quantitatively reacts with var ...[more]

PMID: 29353939

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Project description:CONSPECTUS: Supramolecular assemblies formed from spontaneous self-assembly of amphiphilic macromolecules are explored as biomimetic architectures and for applications in areas such as sensing, drug delivery, and diagnostics. Macromolecular assemblies are usually preferred, compared with their simpler small molecule counterparts, due to their low critical aggregate concentrations (CAC) and high thermodynamic stability. This Account focuses on the structural and functional aspects of assemblies formed from dendrimers, specifically facially amphiphilic dendrons that form micelle or inverse micelle type supramolecular assemblies depending on the nature of the solvent medium. The micelle type assemblies formed from facially amphiphilic dendrons sequester hydrophobic guest molecules in their interiors. The stability of these assemblies is dependent on the relative compatibility of the hydrophilic and hydrophobic functionalities with water, often referred to as hydrophilic-lipophilic balance (HLB). Disruption of the HLB, using an external stimulus, could lead to disassembly of the aggregates, which can then be utilized to cause an actuation event, such as guest molecule release. Studying these possibilities has led to (i) a robust and general strategy for stimulus-induced disassembly and molecular release and (ii) the introduction of a new approach to protein-responsive supramolecular disassembly. The latter strategy provides a particularly novel avenue for impacting biomedical applications. Most of the stimuli-sensitive supramolecular assemblies have been designed to be responsive to factors such pH, temperature, and redox conditions. The reason for this interest stems from the fact that certain disease microenvironments have aberrations in these factors. However, these variations are the secondary imbalances in biology. Imbalances in protein activity are the primary reasons for most, if not all, human pathology. There have been no robust strategies in stimulus-responsive assemblies that respond to these variations. The facially amphiphilic dendrimers provide a unique opportunity to explore this possibility. Similarly, the propensity of these molecules to form inverse micelles in apolar solvents and thus bind polar guest molecules, combined with the fact that these assemblies do not thermodynamically equilibrate in biphasic mixtures, was used to predictably simplify peptide mixtures. The structure-property relationships developed from these studies have led to a selective and highly sensitive detection of peptides in complex mixtures. Selectivity in peptide extraction was achieved using charge complementarity between the peptides and the hydrophilic components present in inverse micellar interiors. These findings will have implications in areas such as proteomics and biomarker detection.

Dataset Information

Multi-Stimuli-Responsive Amphiphilic Assemblies through Simple Postpolymerization Modifications.

Publications

Multi-Stimuli-Responsive Amphiphilic Assemblies through Simple Postpolymerization Modifications.

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