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Chinese Journal of Materials Research  2020, Vol. 34 Issue (6): 452-458    DOI: 10.11901/1005.3093.2019.493
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Preparation of Ultra-fast Temperature Responsive Nanofibrous Hydrogel and Application in Controllable Drug Release
ZHENG Xie1,2, ZHA Liusheng1,2()
1.State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, Shanghai 201620, China
2.College of Materials Science and Engineering, Donghua University, Shanghai 201620, China
Cite this article: 

ZHENG Xie, ZHA Liusheng. Preparation of Ultra-fast Temperature Responsive Nanofibrous Hydrogel and Application in Controllable Drug Release. Chinese Journal of Materials Research, 2020, 34(6): 452-458.

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Abstract  

The nanofibers were firstly prepared by static electrospinning process using the fiber-forming copolymer synthesized from N-isopropylacrylamide and N-methylol acrylamide, and then they were shortened and dispersed in tert-butanol by high-speed stirring. Finally, the shortened nanofibers were assembled into nanofibrous hydrogel with hierarchical porous structure by the processes of freeze drying and followed heat treatment. The resultant nanofibrous hydrogel in aqueous medium holds excellent stability, compression resilience and remarkable temperature-responsiveness. When the temperature of an aqueous medium changed alternately between 20℃ and 55℃, in which the nanofibrous hydrogel reached its swelling- and deswelling-equilibrium state within 34 s and 45 s respectively, exhibiting ultra-fast temperature responsiveness. In vitro drug release experiment results show that when the temperature of the phosphate buffered solution of pH7.4 is altered alternately between 15oC and 47oC the immersed dextran (model drug) loaded nanofibrous hydrogel can controllably release the drug by ''on/off'' mode.

Key words:  organic polymer materials      temperature responsive nanofibrous hydrogel      static electrospinning      controllable drug release     
Received:  25 October 2019     
ZTFLH:  TQ430.50  
Fund: National Natural Science Foundation of China(51373030)

URL: 

https://www.cjmr.org/EN/10.11901/1005.3093.2019.493     OR     https://www.cjmr.org/EN/Y2020/V34/I6/452

Fig.1  1H NMR spectrum of PNN (a) and temperature dependence of light transmittance at the wavelength of 500 nm for the PNN aqueous solution of ca.0.1% (mass fraction) concentration (b)
Fig.2  SEM images of PNN nanofibers with different magnification times (a) low magnification, (b) high magnification
Fig. 3  Optical images of temperature responsive nanofibrous hydrogels with various shapes (a), SEM images of temperature responsive nanofibrous hydrogel at various magnification times (b), optical images of temperature responsive nanofibrous hydrogel in water before and after 300 r/min×24 h oscillation (c), optical images of conventional temperature responsive PNIPAM hydrogel before, during and after compression exerted by a blade (d) and optical images of temperature responsive nanofibrous hydrogel before, during and after compression exerted by a blade (e)
Fig.4  Temperature dependent V/V0 of the nanofibrous hydrogel or the PNIPAM hydrogel (a), time dependent V/V0 of the nanofibrous hydrogel immersed alternately in the aqueous medium of 20℃ or 55℃ (b) and the V/V0 of the nanofibrous hydrogel immersed alternately in the aqueous medium of 20℃ or 55℃ for six cycles (c)
Fig.5  Cumulated drug release profiles obtained from FITC-dextran loaded nanofibrous hydrogel and conventional PNIPAM hydrogel in response to alternating change of temperature between 15 and 47℃
[1] Wei M L, Gao Y F, Li X, et al. Stimuli-responsive polymers and their applications [J]. Polym. Chem., 2017, 8: 127
doi: 10.1039/C6PY01585A
[2] Sánchez-Moreno P, De Vicente J, Nardecchia S, et al. Thermo-sensitive nanomaterials: recent advance in synthesis and biomedical applications [J]. Nanomaterials (Basel), 2018, 8: 935
doi: 10.3390/nano8110935
[3] Matsuo E S, Tanaka T. Kinetics of discontinuous volume–phase transition of gels [J]. J. Chem. Phys., 1988, 89: 1695
[4] Liu Z, Wei J, Faraj Y, et al. Smart hydrogels: network design and emerging applications [J]. Can. J. Chem. Eng., 2018, 96: 2100
doi: 10.1002/cjce.v96.10
[5] Kaneko Y, Nakamura S, Sakai K, et al. Rapid deswelling response of poly (N-isopropylacrylamide) hydrogels by the formation of water release channels using poly (ethylene oxide) graft chains [J]. Macromolecules, 1998, 31: 6099
doi: 10.1021/ma971899g
[6] Zhang G Q, Zha L S, Zhou M H, et al. Rapid deswelling of sodium alginate/poly (N-isopropylacrylamide) semi-interpenetrating polymer network hydrogels in response to temperature and pH changes [J]. Colloid Polym. Sci., 2004, 283: 431
doi: 10.1007/s00396-004-1172-6
[7] Liu G Q, Zha L S, Liang B R. Preparation of fast temperature responsive porous poly (N-isopropylacrylamide) hydrogels using sodium alginate as pore-making agent in sodium chloride solutions [J]. Acta Polym. Sin., 2009, (7): 633
doi: 10.3724/SP.J.1105.2009.00633
(刘高齐, 查刘生, 梁伯润. 在NaCl溶液中以海藻酸钠为致孔剂制备快速温度响应型多孔聚(N-异丙基丙烯酰胺)水凝胶 [J]. 高分子学报, 2009, (7): 633)
doi: 10.3724/SP.J.1105.2009.00633
[8] Xia L W, Xie R, Ju X J, et al. Nano-structured smart hydrogels with rapid response and high elasticity [J]. Nat. Commun., 2013, 4: 2226
doi: 10.1038/ncomms3226 pmid: 23900497
[9] Chen S Y, Wang L Y, Dong X, et al. Fabrication of monodispersed Au@Ag bimetallic nanorod-loaded nanofibrous membrane with fast thermo-responsiveness and its use as a smart free-standing SERS substrate [J]. RSC Adv., 2016, 6: 48479
doi: 10.1039/C6RA04247C
[10] Kim Y J, Ebara M, Aoyagi T. Temperature-responsive electrospun nanofibers for ‘on-off’ switchable release of dextran [J]. Sci. Technol. Adv. Mater., 2012, 13: 064203
doi: 10.1088/1468-6996/13/6/064203 pmid: 27877530
[11] Gil E S, Hudson S M. Stimuli-reponsive polymers and their bioconjugates [J]. Prog. Polym. Sci., 2004, 29: 1173
doi: 10.1016/j.progpolymsci.2004.08.003
[12] Zhang Q S, Zha L S, Ma J H, et al. A novel route to prepare pH- and temperature-sensitive nanogels via a semibatch process [J]. J. Colloid Interface Sci., 2009, 330: 330
doi: 10.1016/j.jcis.2008.09.077 pmid: 19027914
[13] Nagase K, Nagumo Y, Kim M, et al. Local release of VEGF using fiber mats enables effective transplantation of layered cardiomyocyte sheets [J]. Macromol. Biosci., 2017, 17(8). DOI: 10.1002/mabi.201700073
pmid: 28371343
[14] Chen L N, Chiu Y C, Hung J J, et al. Multifunctional electrospun nanofibers prepared from poly ((N-isopropylacrylamide)-co-(N-hydroxymethylacrylamide)) and Their Blends with 1,2-Diaminoanthraquinone for NO gas detection [J]. Macromol. Chem. Phys., 2014, 215: 286
doi: 10.1002/macp.201300604
[15] Naficy S, Brown H R, Razal J M, et al. Spinks a P W. Progress toward robust polymer hydrogels [J]. Aust. J. Chem., 2011, 64: 1007
doi: 10.1071/CH11156
[16] Wang L Y, Chen S Y, Zhou J F, et al. Silver nanoparticles loaded thermoresponsive hybrid nanofibrous hydrogel as a recyclable dip-catalyst with temperature-tunable catalytic activity [J]. Macromol. Mater. Eng., 2017, 302: 1700181
doi: 10.1002/mame.v302.10
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