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J Hazard Mater ; 416: 125897, 2021 08 15.
Artigo em Inglês | MEDLINE | ID: mdl-34492835


Interconnected macro-porous cryogels with robust and pore-tunable structures have been fabricated using chemically crosslinked microfibrillated cellulose (MFC). Periodate oxidation was initially conducted to introduce aldehyde groups into the MFC surface, followed by the freeze-induced chemical crosslinking via the formation of hemiacetal bonds between aldehyde and hydroxyl at -12 °C. The cryogels with pore-tunable structures and sharply enhanced mechanical strengths were finally achieved by re-assembly of MFCs through soaking in NaIO4 solution. Furthermore, the MFC cryogels were post-crosslinked by polyethyleneimine (PEI), bestowing the cryogels with the capability of adsorbing anionic dyes. The stress of the PEI-MFC cryogel at the 80% strain was determined to be 304.5 kPa, which is the maximum value for the nanocellulose-based cryogels reported so far. Finally, the adsorption performances of PEI-MFC cryogels for methyl orange (MO) were evaluated. Maximum adsorption capacity of 500 mg/g could be obtained by the Langmuir model, outperforming that of previous absorbent materials. Reuse experiments indicated that over 90% of adsorption capacity was retained after 6 cycles. Continuous clean-up experiments demonstrated excellent MO removal abilities of the PEI-MFC cryogel. This study shows that the novel, green strategy to fabricate the robust cryogel extends the practical applications of nanocellulose adsorbents for environmental remediation.

Criogéis , Nanofibras , Adsorção , Compostos Azo , Celulose , Corantes , Porosidade
Carbohydr Polym ; 272: 118498, 2021 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-34420751


Construction of monolithic cryogels that can efficiently adsorb proteins is of great significance in biotechnological and pharmaceutical industries. Herein, a novel approach is presented to fabricate microfibrillated cellulose (MFC)/sodium alginate (SA) cryogels by using freezing-induced oxa-Michael reaction at -12 °C. Thanks to the controllable reactiveness of divinyl sulfone (DVS), cryo-concentrated pH increase activates the oxa-Michael reaction between DVS and hydroxyl groups of MFCs and SAs. The obtained composite cryogel exhibits outstanding underwater shape recovery and excellent fatigue resistance. Moreover, the MFC/SAs reveal a high lysozyme adsorption capacity of 294.12 mg/g, surpassing most of absorbent materials previously reported. Furthermore, the cryogel-packed column can purify lysozyme continuously from chicken egg white, highlighting its outstanding practical application performance. Reuse experiments indicated that over 90% of lysozyme extraction capacity was retained after 6 cycles. This work provides a new avenue to design and develop next-generation chromatographic media of natural polysaccharide-based cryogel for protein purification.

J Sep Sci ; 43(16): 3315-3326, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32543754


A novel, facile, and robust strategy was proposed to increase the pore size and mechanical strength of cryogels. By mixing the monomers of acrylamide and 2-hydroxyethyl methacrylate as the precursor, a monolithic copolymer cryogel with large interconnected pores and thick pore walls was prepared. Hydrogen bonding between the two monomers contributed to the entanglement and aggregation of the copolymers, thickening the pore walls and resulting in larger pore sizes. Analysis via mercury porosimetry demonstrated that the interconnected pore diameter of the copolymer cryogel ranged from 10-350 µm, which was far larger than that of the cryogels from one monomer (10-50 µm). Additionally, the thicker pore walls of the copolymer cryogel improved its mechanical strength. Affinity cryogels were prepared through covalent immobilization using Tris(hydroxymethyl)aminomethane as a coupling agent, and the affinity binding of lysozymes on Tris-cryogel was evaluated by the Langmuir isothermal adsorption with the maximum adsorption capacity of 360 mg/g. Compared with that of the Tris-cryogels produced from one monomer, the copolymer Tris-cryogel exhibited higher adsorption capacity and lysozyme purity, when the chicken egg white solution flowed solely driven by gravity. This work provides a new avenue for designing and developing supermacroporous cryogels for bioseparation.

Criogéis/química , Clara de Ovo/química , Muramidase/isolamento & purificação , Adsorção , Animais , Galinhas , Criogéis/síntese química , Estrutura Molecular , Muramidase/química , Muramidase/metabolismo , Tamanho da Partícula , Porosidade , Estresse Mecânico , Propriedades de Superfície
Oncotarget ; 8(46): 80651-80665, 2017 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-29113333


Excessive skin scars due to elective operations or trauma represent a challenging clinical problem. Pathophysiology of hypertrophic scars entails a prolonged inflammatory and proliferative phase of wound healing. Over expression of TGF-ß1 and COX-2 play key regulatory roles of the aberrant fibrogenic responses and proinflammatory mediators. When we silenced TGF-ß1 and COX-2 expression simultaneously in primary human fibroblasts, a marked increase in the apoptotic cell population occurred in contrast to those only treated with either TGF-ß1 or COX-2 siRNA alone. Furthermore, using human hypertrophic scar and skin graft implant models in mice, we observed significant size reductions of the implanted tissues following intra-scar administration of TGF-ß1/COX-2 specific siRNA combination packaged with Histidine Lysine Polymer (HKP). Gene expression analyses of those treated tissues revealed silencing of the target gene along with down regulations of pro-fibrotic factors such as α-SMA, hydroxyproline acid, Collagen 1 and Collagen 3. Using TUNEL assay detection, we found that the human fibroblasts in the implanted tissues treated with the TGF-ß1/COX-2siRNAs combination exhibited significant apoptotic activity. Therefore we conclude that a synergistic effect of the TGF-ß1/COX-2siRNAs combination contributed to the size reductions of the hypertrophic scar implants, through activation of fibroblast apoptosis and re-balancing between scar tissue deposition and degradation.

Int J Pharm ; 494(1): 264-70, 2015 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-26283278


In the present study, a composite system for the controlled and sustained release of hydrophobic/hydrophilic drugs is described. Composite hydrogels were prepared by blending silk fibroin (SF) with PLA-PEG-PLA copolymer under mild aqueous condition. Aspirin and indomethacin were incorporated into SF/Copolymer hydrogels as two model drugs with different water-solubility. The degradation of composite hydrogels during the drug release was mainly caused by the hydrolysis of copolymers. SF with stable ß-sheet-rich structure was not easily degraded which maintained the mechanical integrity of composite hydrogel. The hydrophobic/hydrophilic interactions of copolymers with model drugs would significantly alter the morphological features of composite hydrogels. Various parameters such as drug load, concentration ratio, and composition of copolymer were considered in vitro drug release. Aspirin as a hydrophilic drug could be controlled release from composite hydrogel at a constant rate for 5 days. Its release was mainly driven by diffusion-based mechanism. Hydrophobic indomethacin could be encapsulated in copolymer nanoparticles distributing in the composite hydrogel. Its sustained release was mainly degradation controlled which could last up to two weeks. SF/Copolymer hydrogel has potential as a useful composite system widely applying for controlled and sustained release of various drugs.

Preparações de Ação Retardada/química , Portadores de Fármacos/química , Liberação Controlada de Fármacos , Fibroínas/química , Hidrogéis/química , Polímeros/química , Aspirina/química , Interações Hidrofóbicas e Hidrofílicas , Indometacina/química
J Biomed Mater Res A ; 100(8): 1983-9, 2012 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-22566401


Hydrogels had been prepared by blending PLA-PEG-PLA copolymer with Bombyx mori silk fibroin (SF) solution. Copolymers were synthesized by ring opening polymerization of L-lactide in the presence of dihydroxyl PEG with molar mass of 400 and 1000, and characterized by using (1)H NMR and DSC. Hydrogels formed leaf-like lamellar structures with many nanoglobules which may reserve drugs or growth factors more effectively. Rheological measurements indicated that the adding of copolymer significantly accelerated the hydrogelation of silk fibroin solution which leads to orders-of-magnitude increase in the complex shear modulus to form rigid hydrogel. Hydrogelation kinetics could be controlled easily by changing the concentration ratio, kinds of copolymer and hydrogelation temperature, suggesting the hydrogels could be formed in situ under physiological conditions with suitable mechanical properties. Furthermore, Fourier transform infrared, X-ray diffraction, and differential thermal analysis were employed to study the structure of hydrogels. The copolymer and SF in blend hydrogels were phase separation. There was an increase of ß-sheet content and formation of silk II structure during hydrogelation. These results may indicate that copolymer/SF hydrogels could be a valuable candidate scaffold as in situ-forming hydrogels for drug/growth factor release in tissue engineering.

Fibroínas/química , Hidrogéis/química , Hidrogéis/síntese química , Poliésteres/química , Polietilenoglicóis/química , Absorção , Varredura Diferencial de Calorimetria , Liofilização , Cinética , Microscopia Eletrônica de Varredura , Reologia , Soluções , Espectroscopia de Infravermelho com Transformada de Fourier , Fatores de Tempo , Difração de Raios X