Synthetisch hergestellte, transient thermoresponsive Homopolymere mit einer oberen kritischen Lösungstemperatur für physiologisch relevante Anwendungen

Zhang, Zhiyue; Li, Hui; Kasmi, Sabah; Herck, Simon Van; Deswarte, Kim; Lambrecht, Bart; Hoogenboom, Richard; Nuhn, Lutz; Geest, Bruno G. De

doi:10.1002/ange.201900224

Cited by 4 publications

(2 citation statements)

References 44 publications

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“…Among the few known homopolymers of this type, PNAGA, whose UCST behavior was first characterized by Seuring and Agarwal in 2010, is the most widely studied [92][93][94][95][96]. In addition to UCST-type polymers such as poly(methacrylamide) and polyuracilacrylates, which have been known for some time [51,52], Zhang et al recently presented the synthesis of a novel homopolymer with transiently thermoresponsive behavior [271]. Within a physiologically relevant window, the developed GA-polyHMPA initially exhibits UCST responsiveness, but can subsequently be slowly biodegraded to a fully water-soluble polymer (polyHMPA) via hydrolysis.…”

Section: Ucst Resulting From Strong Hydrogen Bonding Interactionsmentioning

confidence: 99%

Constrained thermoresponsive polymers – new insights into fundamentals and applications

Flemming¹,

Münch²,

Fery³

et al. 2021

Beilstein J. Org. Chem.

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In the last decades, numerous stimuli-responsive polymers have been developed and investigated regarding their switching properties. In particular, thermoresponsive polymers, which form a miscibility gap with the ambient solvent with a lower or upper critical demixing point depending on the temperature, have been intensively studied in solution. For the application of such polymers in novel sensors, drug delivery systems or as multifunctional coatings, they typically have to be transferred into specific arrangements, such as micelles, polymer films or grafted nanoparticles. However, it turns out that the thermodynamic concept for the phase transition of free polymer chains fails, when thermoresponsive polymers are assembled into such sterically confined architectures. Whereas many published studies focus on synthetic aspects as well as individual applications of thermoresponsive polymers, the underlying structure–property relationships governing the thermoresponse of sterically constrained assemblies, are still poorly understood. Furthermore, the clear majority of publications deals with polymers that exhibit a lower critical solution temperature (LCST) behavior, with PNIPAAM as their main representative. In contrast, for polymer arrangements with an upper critical solution temperature (UCST), there is only limited knowledge about preparation, application and precise physical understanding of the phase transition. This review article provides an overview about the current knowledge of thermoresponsive polymers with limited mobility focusing on UCST behavior and the possibilities for influencing their thermoresponsive switching characteristics. It comprises star polymers, micelles as well as polymer chains grafted to flat substrates and particulate inorganic surfaces. The elaboration of the physicochemical interplay between the architecture of the polymer assembly and the resulting thermoresponsive switching behavior will be in the foreground of this consideration.

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Section: Ucst Resulting From Strong Hydrogen Bonding Interactionsmentioning

confidence: 99%

Constrained thermoresponsive polymers – new insights into fundamentals and applications

Flemming¹,

Münch²,

Fery³

et al. 2021

Beilstein J. Org. Chem.

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“…We envision an exciting synergy – between high throughput recombinant synthesis of hybrid biopolymers, characterization of both the kinetics and thermodynamics of their phase behavior, [22] and in‐situ liquid cell electron microscopy [40] – that can exponentially accelerate the pace of bio‐nanomaterials design and discovery. We expect that this strategy will be applicable to other naturally occurring IDPs with UCST behavior, [20e] synthetic polymers, [41] or multi‐component hybrid systems [42] and impact the application of this class of biopolymers for the templated synthesis of nanomaterials at extreme temperatures, responsive reactors and engineered protocells.…”

Section: Discussionmentioning

confidence: 99%

Pathway‐Selection for Programmable Assembly of Genetically Encoded Amphiphiles by Thermal Processing

et al. 2021

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Engineering the fate of supramolecular assemblies by heat treatment (i. e., using thermal preparative pathways) remains challenging and a largely ad hoc process. The rational design of such trajectories requires precise manipulation of the strength of molecularly encrypted interactions along an assembly path defined by changes in free energy as a function of temperature. Here, we use temperature‐triggered liquid–liquid phase separation of proteins to program the nano‐ and mesoscale assembly of a genetically encoded amphiphile – a post‐translationally lipidated protein – along user‐defined thermal trajectories. This molecularly defined pathway was used to funnel thermal energy into the system to direct building blocks to a previously inaccessible region of the energy landscape, and to synthesize two‐dimensional nanomaterials with sophisticated structures, such as braids and toroids. Because proteins’ phase boundaries and transition are programmable at the sequence‐level, our strategy opens new horizons to expand the structural hierarchy and functional landscape of protein‐based materials.

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Macromolecular Isomerism in Giant Molecules

Shao

Shen

Zhang

2020

Chemistry A European J

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Macromolecular isomerism has been an important yet largely understudied subject. Giant molecules based on molecular nanoparticles exhibit properties highly dependent on the primary structures, providing a platform for such studies. Various isomers have been designed, synthesized and characterized, including sequence‐, regio‐, and topo‐isomers. The self‐assembly of these isomers is influenced by the distinct symmetry and collective interaction of each building block in a subtle and delicate way. The results suggest that isomerism may be exploited as a new way for fine‐tuning the structures and properties of macromolecules, which should be of great interest in both fundamental research and technical innovation.

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Synthetisch hergestellte, transient thermoresponsive Homopolymere mit einer oberen kritischen Lösungstemperatur für physiologisch relevante Anwendungen

Cited by 4 publications

References 44 publications

Constrained thermoresponsive polymers – new insights into fundamentals and applications

Constrained thermoresponsive polymers – new insights into fundamentals and applications

Pathway‐Selection for Programmable Assembly of Genetically Encoded Amphiphiles by Thermal Processing

Macromolecular Isomerism in Giant Molecules

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