Redox-Controlled Voltage Responsive Micelles Assembled by Noncovalently Grafted Polymers for Controlled Drug Release

Yuan, Zhenyu; Wang, Jie; Wang, Yiming; Zhong, Yujie; Zhang, Xinsheng; Li, Li; Wang, Junyou; Lincoln, Stephen F.; Guo, Xuhong

doi:10.1021/acs.macromol.8b02641

Cited by 47 publications

(28 citation statements)

References 58 publications

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“…DPA is a well‐known ligand for lanthanide ions, and the characteristic sharp‐lines of the Eu(III) emission at 615 nm after excitation of DPA at 280 nm (antenna effect) corroborate that βCD‐DPA coordinates to the metal ion (Figure S6). The host‐guest interaction between βCD and adamantane has been extensively demonstrated previously, so Ad‐SS‐Ad molecules were designed to link two coordination complexes, driving the formation of branched oligomeric structures. By adding a block copolymer (P2MVP 128 ‐b‐PEO 477 ) composed of a positively‐charged part and a neutral part to the negatively‐charged oligomeric units, Ad‐SS‐Ad‐based C4Ms were formed, (Figure S10).…”

Section: Resultsmentioning

confidence: 92%

Assembly, Disassembly and Reassembly of Complex Coacervate Core Micelles with Redox‐Responsive Supramolecular Cross‐Linkers

et al. 2020

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Polymer-based micellar assemblies are gaining increasing attention in the smart materials field, yet the design of micelles that show redox-responsive disassembly and, e. g., cargo release is still a challenge. To form redox-responsive micelles, we developed cyclodextrin-based coacervate core micelles that form under interplay of four orthogonal interactions: multivalent electrostatic coacervation, metal-to-ligand coordination chemistry, supramolecular host-guest interactions, and a reversible covalent disulfide metal-complex crosslinker. The cleavage of this crosslinker by dithiotreithol results in the breaking of oligomeric europium(III) structures in the core and results in the disassembly of the 70 nm size micelles. Over hours, due to the oxidation of thiolates to disulfides, monomeric units can recrosslink into oligomeric core-units, favoring micellar reassembly. The time required to reassemble can be controlled by varying the reducing agent concentration or the ratio between redox-responsive and non-redox-responsive crosslinkers. Controlled Methyl Red encapsulation and release indicate the potential of these micelles, for, e. g., controlled drug uptake and delivery.

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Section: Resultsmentioning

confidence: 92%

Assembly, Disassembly and Reassembly of Complex Coacervate Core Micelles with Redox‐Responsive Supramolecular Cross‐Linkers

et al. 2020

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“…The results suggested that the supramolecular ion assembly between β-CD and Fc would be beneficial to the mechanical properties of the hydrogels. The supramolecular ion assembly of a copolymer containing β-CD and Fc moieties has also been studied and the redox-switchable properties of the copolymer have been confirmed in the electrochemical response of the Fc moieties [41], conferring voltage-controllable assembly and disassembly features to the samples [42].…”

Section: Introductionmentioning

confidence: 98%

Supramolecular ionic polymer/carbon nanotube composite hydrogels with enhanced electromechanical performance

Zhang

Chen

et al. 2020

Nanotechnology Reviews

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AbstractElectroactive hydrogels have received increasing attention due to the possibility of being used in biomimetics, such as for soft robotics and artificial muscles. However, the applications are hindered by the poor mechanical properties and slow response time. To address these issues, in this study, supramolecular ionic polymer–carbon nanotube (SIPC) composite hydrogels were fabricated via in situ free radical polymerization. The polymer matrix consisted of carbon nanotubes (CNTs), styrene sulfonic sodium (SSNa), β-cyclodextrin (β-CD)-grafted acrylamide, and ferrocene (Fc)-grafted acrylamide, with the incorporation of SSNa serving as the ionic source. On applying an external voltage, the ions accumulate on one side of the matrix, leading to localized swelling and bending of the structure. Therefore, a controllable and reversible actuation can be achieved by changing the applied voltage. The tensile strength of the SIPC was improved by over 300%, from 12 to 49 kPa, due to the reinforcement effect of the CNTs and the supramolecular host–guest interactions between the β-CD and Fc moieties. The inclusion of CNTs not only improved the tensile properties but also enhanced the ion mobility, which lead to a faster electromechanical response. The presented electro-responsive composite hydrogel shows a high potential for the development of robotic devices and soft smart components for sensing and actuating applications.

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“…The unique electrochemical, physicochemical, magnetic, and optical properties of ferrocene (Fc)‐containing polymers have attracted widespread concerns in the fields of molecular battery, amperometric biosensors, sensors, nanopatterns, drug delivery, electrochromics, and catalysis . Particularly, Fc‐containing polymers could be used as reducing agents to prepare MNPs .…”

Section: Introductionmentioning

confidence: 99%

AuNPs composites of gelatin hydrogels crosslinked by ferrocene‐containing polymer as recyclable supported catalysts

Long

Song

Shi

et al. 2019

J of Applied Polymer Sci

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To fabricate a recyclable supported catalyst based on gold nanoparticles (AuNPs) and gelatin hydrogel (HG) composites, a ferrocene (Fc)-containing tetrablock copolymer [P(NCHO-b-NFc-b-NTEG-b-NCHO)] was used as both reducing and stabilizing agents for AuNPs and as a crosslinker for HG. First, the effects of Fc-containing polymers, including homopolymer PNFc and copolymer P(NCHO-b-NFc-b-NTEG-b-NCHO), and different solvent systems on the morphology and aggregation of AuNPs were examined by using ultraviolet-visible spectroscopy, transmission electron microscopy, and dynamic light scattering. Second, two strategies (blending and soaking) were applied to prepare different AuNPs/HG composites (AuNPs-HG), and their structure and properties were studied by using various techniques including scanning electron microscopy, X-ray diffraction, and thermogravimetry. Finally, the catalytic performance and reusability of AuNPs-HG-1 (via blending) and AuNPs-HG-2 (via soaking) were evaluated utilizing the model catalytic reduction of 4-nitrophenol to 4-aminophenol by NaBH 4 . Results indicated that P(NCHO-b-NFc-b-NTEG-b-NCHO) dissolved in N,Ndimethylformamide was the optimal reductant and stabilizer to prepare AuNPs. The in situ reduction of Au III ions to Au 0 particles was very essential for the fabrication of AuNPs-HG in terms of hydrogel pore size, Au 0 distribution and immobilization stability, and hydrogel thermal stability. Due to the stronger interactions among AuNPs, P(NCHO-b-NFc-b-NTEG-b-NCHO), and gelatin molecules in the blending strategy, AuNPs-HG-1 showed better mechanical stability and catalytic performance and more reusing cycles than AuNPs-HG-2. This work highlights the design and fabrication of robust recyclable supported AuNP catalyst by using eco-friendly Fccontaining HGs.

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Redox-Controlled Voltage Responsive Micelles Assembled by Noncovalently Grafted Polymers for Controlled Drug Release

Cited by 47 publications

References 58 publications

Assembly, Disassembly and Reassembly of Complex Coacervate Core Micelles with Redox‐Responsive Supramolecular Cross‐Linkers

Assembly, Disassembly and Reassembly of Complex Coacervate Core Micelles with Redox‐Responsive Supramolecular Cross‐Linkers

Supramolecular ionic polymer/carbon nanotube composite hydrogels with enhanced electromechanical performance

AuNPs composites of gelatin hydrogels crosslinked by ferrocene‐containing polymer as recyclable supported catalysts

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