Self-Assembled Micelles from Thermoresponsive Poly(methyl methacrylate)-<i>b</i>-poly(<i>N</i>-isopropylacrylamide) Diblock Copolymers in Aqueous Solution

Henschel, Cristiane; Meledam, Geethu P.; Schroer, Martin A.; Müller‐Buschbaum, Peter; Laschewsky, André; Papadakis, Christine M.

doi:10.1021/acs.macromol.0c02189

Cited by 22 publications

(55 citation statements)

References 63 publications

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“…Poly( N -vinylcaprolactam) (PVCL) has received significant attention due to its characteristic features and diversified applications in biomedical science and pharmaceutical industries. − Owing to its tremendous sensitivity and biocompatibility, PVCL-based “smart” materials such as nanohybrids, microgels, hydrogels, and copolymers have been widely used in various applications. ,− PVCL can respond to different stimulants, such as proteins, temperature, ionic strength, and osmolytes. − Deep eutectic solvents (DESs) are an emerging class of benign liquid formulations that have gained popularity owing to idiosyncratic properties that outperform traditional ionic liquids (ILs). − High solubilization power, solventless preparation, low volatility, good stability, cost effectiveness, and wider availability are some of the properties of DESs that make them an ingenious and perfect solvent alternative. − The DESs consist of hydrogen bond acceptor (HBA) and hydrogen bond donor (HBD) groups.…”

Section: Introductionmentioning

confidence: 99%

Tweaking Behavior of Hydrogen Bond Donor in Choline Chloride-Based Deep Eutectic Solvents for Regulating the Phase Transition of Poly(N-vinylcaprolactam): A Sustainable Medium for an Early Hydrophobic Collapse

Kumar

Umapathi

Bisht

et al. 2021

ACS Sustainable Chem. Eng.

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Deep eutectic solvents (DESs) are recognized as a "green" alternative to conventional ionic liquids and organic solvents owing to their specific properties. In this study, the influence of DESs containing choline chloride (ChCl) as a hydrogen bond acceptor (HBA) and urea, ethylene glycol (EG), and lactic acid (LA) as hydrogen bond donors (HBD) on the thermoresponsive behavior of poly(N-vinylcaprolactam) (PVCL) is investigated using various techniques. Spectroscopic investigations indicate biased interactions of the HBD group present in the DESs with a hydration layer of PVCL. Dynamic light scattering and temperature-dependent fluorescence spectroscopy results clearly show a decrease in the lower critical solution temperature of PVCL in the presence of the DESs. The hydrophobic collapse of PVCL in the presence of the DESs follows the order ChCl:urea > ChCl:EG > ChCl:LA. It is proposed that the presence of DESs does not interfere with the functional groups present in PVCL; however, it ruptures the hydrogen bonding between PVCL and the water molecules and destabilizes the water gradient around PVCL. The DESs have provided an alternative platform for low-temperature dehydration of PVCL, which can be useful as a drug carrier agent.

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Section: Introductionmentioning

confidence: 99%

Tweaking Behavior of Hydrogen Bond Donor in Choline Chloride-Based Deep Eutectic Solvents for Regulating the Phase Transition of Poly(N-vinylcaprolactam): A Sustainable Medium for an Early Hydrophobic Collapse

Kumar

Umapathi

Bisht

et al. 2021

ACS Sustainable Chem. Eng.

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“…4C , Table 1 , and table S1). Like in all thermosensitive polymers ( 54 , 55 ), onset of gelation shifts to lower temperatures with increasing solution concentration ( Fig. 4C ).…”

Section: Resultsmentioning

confidence: 69%

Injectable bottlebrush hydrogels with tissue-mimetic mechanical properties

et al. 2022

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Injectable hydrogels are desired in many biomedical applications due to their minimally invasive deployment to the body and their ability to introduce drugs. However, current injectables suffer from mechanical mismatch with tissue, fragility, water expulsion, and high viscosity. To address these issues, we design brush-like macromolecules that concurrently provide softness, firmness, strength, fluidity, and swellability. The synthesized linear-bottlebrush-linear (LBL) copolymers facilitate improved injectability as the compact conformation of bottlebrush blocks results in low solution viscosity, while the thermoresponsive linear blocks permit prompt gelation at 37°C. The resulting hydrogels mimic the deformation response of supersoft tissues such as adipose and brain while withstanding deformations of 700% and precluding water expulsion upon gelation. Given their low cytotoxicity and mild inflammation in vivo, the developed materials will have vital implications for reconstructive surgery, tissue engineering, and drug delivery applications.

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“…[ 48,49 ] This best model fit is established on several key structural parameters consisting of the radius of gyration ( r g ), a shape factor ( s ), and Porod exponent ( m ). [ 50,51 ] The determined values are 20.0 ± 1.2 nm, 0.83 ± 0.01 and 1.00 ± 0.02, respectively. Consequently, a rigidly rod‐like shape can be applied to describe the generated PS‐ b ‐PEO aggregates, and the length is calculated to be ≈15.5 nm.…”

Section: Resultsmentioning

confidence: 89%

Morphology Transformation Pathway of Block Copolymer‐Directed Cooperative Self‐Assembly of ZnO Hybrid Films Monitored In Situ during Slot‐Die Coating

Tian

Yin

et al. 2021

Adv Funct Materials

Self Cite

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Cooperative self-assembly (co-assembly) of diblock copolymers (DBCs) and inorganic precursors that takes inspiration from the rich phase separation behavior of DBCs can enable the realization of a broad spectrum of functional nanostructures with the desired sizes. In a DBC assisted sol-gel chemistry approach with polystyrene-block-poly(ethylene oxide) and ZnO, hybrid films are formed with slot-die coating. Pure DBC films are printed as control. In situ grazing-incidence small-angle X-ray scattering measurements are performed to investigate the self-assembly and co-assembly process during the film formation. Combining complementary ex situ characterizations, several distinct regimes are differentiated to describe the morphological transformations from the initially solvent-dispersed to the ultimately solidified films. The comparison of the assembly pathway evidences that the key step in the establishment of the pure DBC film is the coalescence of spherical micelles toward cylindrical domains. Due to the presence of the phase-selective precursor, the formation of cylindrical aggregates in the solution is crucial for the structural development of the hybrid film. The pre-existing cylinders in the ink impede the domain growth of the hybrid film during the subsequent drying process. The precursor reduces the degree of order, prevents crystallization of the PEO block, and introduces additional length scales in the hybrid films.

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Self-Assembled Micelles from Thermoresponsive Poly(methyl methacrylate)-b-poly(N-isopropylacrylamide) Diblock Copolymers in Aqueous Solution

Cited by 22 publications

References 63 publications

Tweaking Behavior of Hydrogen Bond Donor in Choline Chloride-Based Deep Eutectic Solvents for Regulating the Phase Transition of Poly(N-vinylcaprolactam): A Sustainable Medium for an Early Hydrophobic Collapse

Tweaking Behavior of Hydrogen Bond Donor in Choline Chloride-Based Deep Eutectic Solvents for Regulating the Phase Transition of Poly(N-vinylcaprolactam): A Sustainable Medium for an Early Hydrophobic Collapse

Injectable bottlebrush hydrogels with tissue-mimetic mechanical properties

Morphology Transformation Pathway of Block Copolymer‐Directed Cooperative Self‐Assembly of ZnO Hybrid Films Monitored In Situ during Slot‐Die Coating

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