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The architectural change of the shell forming block from linear to V-shaped accelerates micellar disassembly but slows the complete enzymatic degradation of the amphiphiles

DOI: 10.1021/acs.biomac.0c00882 DOI Help

Authors: Merav Segal (Tel-Aviv University) , Lihi Ozery (Tel Aviv University) , Gadi Slor (Tel Aviv University) , Shreyas Shankar Wagle (Tel Aviv University) , Tamara Ehm (Tel Aviv University; Ludwig- Maximilians-Universit√§t M√ľnchen) , Roy Beck (Tel-Aviv University) , Roey J. Amir (Tel Aviv University)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Biomacromolecules

State: Published (Approved)
Published: August 2020
Diamond Proposal Number(s): 24693

Abstract: Tuning the enzymatic degradation and disassembly rates of polymeric amphiphiles and their assemblies is crucial for designing enzyme-responsive nanocarriers for controlled drug delivery applications. The common methods to control the enzymatic degradation of amphiphilic polymers are to tune the molecular weights and ratios of the hydrophilic and hydrophobic blocks. In addition, to these approaches, the architecture of the hydrophilic block can also serve as a tool to tune enzymatic degradation and disassembly. To gain deeper understanding of the effect of the molecular architecture of the hydrophilic block we prepared two types of well-defined PEG-dendron amphiphiles bearing linear or V-shaped PEG chains as the hydrophilic blocks. The high molecular precision of these amphiphiles, which emerges from the utilization of dendrons as the hydrophobic blocks allowed us to study the self-assembly and enzymatic degradation and disassembly of the two types of amphiphiles with high resolution. Interestingly, the micelles of the V-shaped amphiphiles were significantly smaller and disassembled faster than those of the amphiphiles based on linear PEG. However, the complete enzymatic cleavage of the hydrophobic end-groups was significantly slower for the V-shaped amphiphiles. Our results show that the V-shape architecture can stabilize the unimer state and hence plays a double role in the enzymatic degradation and the induced disassembly and how it can be utilized to control the release of encapsulated or bound molecular cargo.

Journal Keywords: Stimuli-responsive; polymeric amphiphiles; dendrimers

Subject Areas: Chemistry, Biology and Bio-materials, Medicine


Instruments: B21-High Throughput SAXS

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