Tunable, concentration‐independent, sharp, hysteresis‐free UCST phase transition from poly(<i>N</i>‐acryloyl glycinamide‐acrylonitrile) system

Käfer, Florian; Lerch, Arne; Agarwal, Seema

doi:10.1002/pola.28374

Cited by 36 publications

(38 citation statements)

References 33 publications

(66 reference statements)

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“…The latter contain H‐donor and H‐acceptor sites, which are able to form intra‐molecular reversible hydrogen bonds (globule conformation below UCST) and inter‐molecular bonds with water (coil conformation above UCST). [ 11–21 ] The non‐ionic polymers have attracted a great deal of attention due to their insensitivity to salts, which make them more attractive for applications in physiological environment. [ 22–24 ] During the last decade, efforts have been focused toward developing novel water‐soluble copolymers exhibiting UCST behavior by copolymerizing H‐donor monomers ( N ‐acryloyl glycinamide [ 11–16 ] or acrylamide [ 15,17–21,25 ] ) and H‐acceptor monomers (acrylonitrile, [ 11,15,18,19,21,25,26 ] styrene, [ 15,17 ] and butyl acrylate [ 15 ] ).…”

Section: Figurementioning

confidence: 99%

“…[ 11–21 ] The non‐ionic polymers have attracted a great deal of attention due to their insensitivity to salts, which make them more attractive for applications in physiological environment. [ 22–24 ] During the last decade, efforts have been focused toward developing novel water‐soluble copolymers exhibiting UCST behavior by copolymerizing H‐donor monomers ( N ‐acryloyl glycinamide [ 11–16 ] or acrylamide [ 15,17–21,25 ] ) and H‐acceptor monomers (acrylonitrile, [ 11,15,18,19,21,25,26 ] styrene, [ 15,17 ] and butyl acrylate [ 15 ] ). Such (co)polymers have been mainly prepared using free radical polymerization [ 11,14–17,26 ] and by thermally initiated controlled radical polymerization such as atom transfer radical polymerization [ 13 ] and reversible addition fragmentation chain transfer (RAFT) [ 11,12,16–19,25 ] The impacts of various parameters on the UCST phase transition, including salts, pH, molecular weight, molecular weight distribution, and chemical composition, have been well evaluated.…”

Section: Figurementioning

confidence: 99%

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Synthesis of Thermoresponsive Copolymers with Tunable UCST‐Type Phase Transition Using Aqueous Photo‐RAFT Polymerization

Lertturongchai

Ibrahim

Durand

et al. 2020

Macromol. Rapid Commun.

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H-acceptor sites, which are able to form intra-molecular reversible hydrogen bonds (globule conformation below UCST) and inter-molecular bonds with water (coil conformation above UCST). [11][12][13][14][15][16][17][18][19][20][21] The non-ionic polymers have attracted a great deal of attention due to their insensitivity to salts, which make them more attractive for applications in physiological environment. [22][23][24] During the last decade, efforts have been focused toward developing novel water-soluble copolymers exhibiting UCST behavior by copolymerizing H-donor monomers (N-acryloyl glycinamide [11][12][13][14][15][16] or acrylamide [15,[17][18][19][20][21]25] ) and H-acceptor monomers (acrylonitrile, [11,15,18,19,21,25,26] styrene, [15,17] and butyl acrylate [15] ). Such (co)polymers have been mainly prepared using free radical polymerization [11,[14][15][16][17]26] and by thermally initiated controlled radical polymerization such as atom transfer radical polymerization [13] and reversible addition fragmentation chain transfer (RAFT) [11,12,[16][17][18][19]25] The impacts of various parameters on the UCST phase transition, including salts, pH, molecular weight, molecular weight distribution, and chemical composition, have been well evaluated. [7][8][9]25,27] However, such studies were carried out at low polymer concentrations (below 5 wt%). This could induce, an unintentional confusion between the UCST and the apparent cloud point temperature (T CP ), which refers to the temperature at which the phase transition occurs depending on the investigated concentration level. The UCST of a given polymer in solution is obtained from an isobaric phase diagram where T CP are plotted versus the polymer concentrations. [7][8][9] T CP should increase with the polymer concentrations up to a maximum temperature, called UCST, before going down again.In this context, we envisioned to use aqueous photo-mediated RAFT (photo-RAFT) polymerization that would be able to prepare well-controlled UCST-type copolymers directly in water at very high concentration. Although photo-RAFT [28][29][30][31][32][33] has grasped great interests due to its versatility, rapidity, and ability to produce well-controlled polymers, it has never been employed for the synthesis of UCST-type polymers. This study provides new insight into UCST-type copolymers and aims to develop facile approach to investigate such kind of thermoresponsive behavior, less described in the literature currently.

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Section: Figurementioning

confidence: 99%

Section: Figurementioning

confidence: 99%

Synthesis of Thermoresponsive Copolymers with Tunable UCST‐Type Phase Transition Using Aqueous Photo‐RAFT Polymerization

Lertturongchai

Ibrahim

Durand

et al. 2020

Macromol. Rapid Commun.

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“…Hydrolysis of the amide group of PNAGA and use of ionic initiators in radical polymerization are other factors, which contribute in suppressing the UCST behavior of polymer [42]. However, it has been observed that polymer concentration in solution affects the UCST, and therefore Käfer et al [44] synthesized a copolymer of PNAGA using AN as second block (Figure 9) to avoid the effect of concentration and to retain narrow cooling/ heating hysteresis in water. The T pt of copolymer P(NAGA-co-AN) was found to be independent of polymer concentration, and can be easily tuned by altering the AN content in copolymer.…”

Section: Poly(n-acryloylglycinamide)mentioning

confidence: 99%

“…Copolymerization of N-acryloyl glycinamide and acrylonitrile by using cyanomethyl dodecyl trithiocarbonate (CMDT) as chain transfer agent and 2,2´-Azoisobutyronitrile (AIBN) as initiator[44].…”

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confidence: 99%

Advances in thermo-responsive polymers exhibiting upper critical solution temperature (UCST)

Bansal¹,

Upadhyay²,

Saraogi³

et al. 2019

Express Polym. Lett.

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Immense work has been conducted in the field of thermoresponsive polymers specifically of lower critical solution temperature (LCST) type, but upper critical solution temperature (UCST) type polymers remain a significantly unexplored domain. However, in recent years, UCST polymers have attracted increased attention as evidenced by the rise in publications in the same domain, and therefore, this review is an attempt to compile the reported UCST-type polymers. Unlike LCST, UCST polymers are insoluble at low temperature but solubilize in a given solvent as the temperature increases. The synthesis approaches and applications of reported UCST polymers are discussed in this article. Emphasis has been given to the polymers exhibiting UCST behavior in aqueous medium, due to the obvious advantage of their wide applicability. It is quite apparent from this study that the attempts to synthesize novel polymers and copolymers exhibiting UCST has faced an upsurge, but their application part still requires considerable attention. Figure 4. (a) Representative structure of poly(acrylamide-co-acrylonitrile) and (b) turbidity cooling curves of poly(AAmco-AN) with different acrylonitrile content in mole% (numbers in graph). Reproduced with permission from [33],

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“…The biomedical applications of UCST polymers are strongly impeded due to the sensitivity to ionic strengths and polymer concentrations as most of the UCST polymers were based on polyzwitterions . Recently, we synthesized a series of noncharged UCST‐type polymers with tunable cloud points based on copolymers of N ‐acryloylglycinamide and acrylonitrile, which were independent on ionic strengths and polymer concentrations . Block and graft copolymers of noncharged UCST‐type segments with hydrophilic poly(ethylene glycol), poly(dimethylacrylamide), and poly( N , N ‐dimethylaminoethyl methacrylate) provide temperature dependent micellar structures which opens up an interesting future direction of thermoresponsive polymers in biomedical applications .…”

Section: Introductionmentioning

confidence: 99%

Let There be Light: Polymeric Micelles with Upper Critical Solution Temperature as Light‐Triggered Heat Nanogenerators for Combating Drug‐Resistant Cancer

Deng

Käfer

Chen

et al. 2018

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Complete drug release and efficient drug retention are two critical factors in reversing drug resistance in cancer therapy. In this regard, polymeric micelles with an upper critical solution temperature (UCST) are designed as a new exploration to reverse drug resistance. The amphiphilic UCST-type block copolymers are used to encapsulate photothermal agent IR780 and doxorubicin (DOX) simultaneously. The integrated UCST-type drug nanocarriers show light-triggered multiple synergistic effects to reverse drug resistance and are expected to kill three birds with one stone: First, owing to the photothermal effect of IR780, the nanocarriers will be dissociated upon exposure to laser irradiation, leading to complete drug release. Second, the photothermal effect-induced hyperthermia is expected to avoid the efflux of DOX and realize efficient drug retention. Last but not least, photothermal ablation of cancer cells can be achieved after laser irradiation. Therefore, the UCST-type drug nanocarriers provide a new strategy in reversing drug resistance in cancer therapy.

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Tunable, concentration‐independent, sharp, hysteresis‐free UCST phase transition from poly(N‐acryloyl glycinamide‐acrylonitrile) system

Cited by 36 publications

References 33 publications

Synthesis of Thermoresponsive Copolymers with Tunable UCST‐Type Phase Transition Using Aqueous Photo‐RAFT Polymerization

Synthesis of Thermoresponsive Copolymers with Tunable UCST‐Type Phase Transition Using Aqueous Photo‐RAFT Polymerization

Advances in thermo-responsive polymers exhibiting upper critical solution temperature (UCST)

Let There be Light: Polymeric Micelles with Upper Critical Solution Temperature as Light‐Triggered Heat Nanogenerators for Combating Drug‐Resistant Cancer

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