Thermo-reversible sol–gel transition of aqueous solutions of patchy polymers

Parmar, Indravadan A.; Shedge, Aarti S.; Badiger, Manohar V.; Wadgaonkar, Prakash P.; Lele, Ashish

doi:10.1039/c6ra27030a

Cited by 17 publications

(12 citation statements)

References 79 publications

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“…Polymers have been used in theranostics for a long time. Their abilities to form a gel and exhibit sol-gel transition have been exploited in many fields ( 12 , 13 ). Polymers are often used as carriers in many targeted drug therapies that require shielding from the immune system and enzymatic degradation.…”

Section: Introductionmentioning

confidence: 99%

Nanohybrids as Protein-Polymer Conjugate Multimodal Therapeutics

Kiran

Khan

Neekhra

et al. 2021

Front. Med. Technol.

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Protein therapeutic formulations are being widely explored as multifunctional nanotherapeutics. Challenges in ensuring susceptibility and efficacy of nanoformulation still prevail owing to various interactions with biological fluids before reaching the target site. Smart polymers with the capability of masking drugs, ease of chemical modification, and multi-stimuli responsiveness can assist controlled delivery. An active moiety like therapeutic protein has started to be known as an important biological formulation with a diverse medicinal prospect. The delivery of proteins and peptides with high target specificity has however been tedious, due to their tendency to aggregate formation in different environmental conditions. Proteins due to high chemical reactivity and poor bioavailability are being researched widely in the field of nanomedicine. Clinically, multiple nano-based formulations have been explored for delivering protein with different carrier systems. A biocompatible and non-toxic polymer-based delivery system serves to tailor the polymer or drug better. Polymers not only aid delivery to the target site but are also responsible for proper stearic orientation of proteins thus protecting them from internal hindrances. Polymers have been shown to conjugate with proteins through covalent linkage rendering stability and enhancing therapeutic efficacy prominently when dealing with the systemic route. Here, we present the recent developments in polymer-protein/drug-linked systems. We aim to address questions by assessing the properties of the conjugate system and optimized delivery approaches. Since thorough characterization is the key aspect for technology to enter into the market, correlating laboratory research with commercially available formulations will also be presented in this review. By examining characteristics including morphology, surface properties, and functionalization, we will expand different hybrid applications from a biomaterial stance applied in in vivo complex biological conditions. Further, we explore understanding related to design criteria and strategies for polymer-protein smart nanomedicines with their potential prophylactic theranostic applications. Overall, we intend to highlight protein-drug delivery through multifunctional smart polymers.

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Section: Introductionmentioning

confidence: 99%

Nanohybrids as Protein-Polymer Conjugate Multimodal Therapeutics

Kiran

Khan

Neekhra

et al. 2021

Front. Med. Technol.

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“…By modifying a high molecular weight precursor copolymer comprising N,Ndimethylacrylamide and acrylic acid with hydrophobic moieties of n-dodecyl amine an inverse thermogelling hydrogel could be realized. 22 At 0 °C, a viscosity of ca. 1 kPa*s could be obtained by varying the sol/gel temperature with different polymer concentrations.…”

Section: Introductionmentioning

confidence: 99%

An Inverse Thermogelling Bioink Based on an ABA Type Poly(2-Oxazoline) Amphiphile

Hahn¹,

Karakaya²,

Zorn³

et al. 2021

Preprint

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Hydrogels are key components in several biomedical research areas such as biofabrication. Here, a novel ABA-type triblock copolymer is introduced that undergoes a inverse thermogelation, i.e. it forms a hydrogel about cooling aqueous polymer solutions. The macroporous hydrogel was rheologically investigate in detail and used for 3D printing using an extrusion based printer. Preliminary experiment show very good cytocompatibility of NIH 3T3 cells also after printing and the possibility to combine the novel material with other hydrogel forming materials such as alginate.<br>

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“…15 In addition, Lele and co-workers described hydrophobically modified copolymers that undergo inverse thermogelation. 16 All these known systems have in common that intermolecular and intramolecular hydrogen bonding between polymer repeat units can occur, which is indeed the main driving force for the UCST phenomenon in general. In stark contrast, A-pPheOzi-A cannot undergo such hydrogen bonding between repeat units and neither pMeOx nor pPheOzi are thermoresponsive per se.…”

Section: Introductionmentioning

confidence: 99%

Unravelling a novel mechanism in polymer self-assemblies: An order-order transition based on molecular interactions between hydrophilic and hydrophobic polymer blocks

Hahn¹,

Zorn²,

Kehrein³

et al. 2021

Preprint

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Thermoresponsive hydrogel formation upon cooling in aqueous media is rarely described for synthetic polymers in the literature. However, if the sol-gel transition occurs in the physiologically relevant range (0-40 °C), there are many possible applications in areas such as drug delivery and biofabrication. Here, we describe a new mechanism of a thermally induced order-order transition in polymer self-assembly of an ABA triblock consisting of hydrophilic A blocks and a hydrophobic aromatic B block. Small-angle X-ray scattering confirmed worm-to-sphere transition upon heating on the nanoscale level while wide-angle X-ray scattering indicated a more uniform ordering of the macromolecular chains on the scale of 4-7 Å. NMR spectroscopy showed reduced mobility of various polymer segments in the hydrogel state, especially in the hydrophobic aromatic region. More importantly however, solution and solid-state NMR investigations also revealed close proximity of hydrophobic and hydrophilic repeat units in the gel state, which is less pronounced in the sol state. This interaction between the hydrophilic and hydrophobic block is responsible for the order-order transition and –ipso facto– inverse thermogelation. This unusual interaction is supported in silico by molecular dynamics modeling. Changes in the structure of the hydrophilic A blocks can be used to tune the gel strength, persistence, and gelation kinetics. This order-order transition based on unexpected and previously not described interactions between the hydrophilic and the hydrophobic repeat units opens new avenues to control and design macromolecular self-assembly.

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Thermo-reversible sol–gel transition of aqueous solutions of patchy polymers

Cited by 17 publications

References 79 publications

Nanohybrids as Protein-Polymer Conjugate Multimodal Therapeutics

Nanohybrids as Protein-Polymer Conjugate Multimodal Therapeutics

An Inverse Thermogelling Bioink Based on an ABA Type Poly(2-Oxazoline) Amphiphile

Unravelling a novel mechanism in polymer self-assemblies: An order-order transition based on molecular interactions between hydrophilic and hydrophobic polymer blocks

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