ACS Applied Materials & Interfaces
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2023
·
IF 9.5
Qing Li,Xinke Yu,Shiqi Zhang,Mengyue Xu,Yunyi Yang,Zhili Wan,Xiaoquan Yang
Supramolecular hydrogels self-assembled from naturally occurring small molecules (e.g., glycyrrhizic acid, GA) are promising materials for controlled bioactive delivery due to their facile fabrication processes, excellent biocompatibility, and versatile stimuli-responsive behaviors. However, most of these natural hydrogels suffer from poor mechanical strength and processability for practical applications. In this work, through adopting a multicomponent gel approach, we developed a novel mechanically robust GA-based hydrogel with an interpenetrating double network (DN) that is composed of a Ca2+-enhanced hydrogen-bond supramolecular GA nanofibril (GN) network and a Ca2+cross-linked natural polysaccharide sodium alginate (ALG) network. Compared to the single GN network (SN) hydrogel, the GN-ALG hybrid hydrogels (GN-ALG-DN) with the hierarchical double-network structure possess excellent mechanical properties and shaping adaptation, encouraging small and large amplitude oscillatory shear (SAOS and LAOS) rheological performances, better thermal stability, higher resistance to large compression deformations, and lower swelling behaviors. Furthermore, the GN-ALG-DN hydrogels exhibit a pH-responsive and sustained release behavior of nutrients (i.e., vitamin B12, VB12), showing a faster VB12 release rate with a higher swelling ratio in an alkaline condition (pH 7.5) than in an acidic condition (pH 2.5). This is ascribed to the fact that the higher dissociation degree of carboxylic groups in GA and ALG molecules in an alkaline environment induces the erosion and looseness of the self-assembled GN network and the ionic-cross-linked ALG network, which can lead to the decomposition of the hybrid hydrogels and thereby increases the release of nutrients. Cytotoxicity tests further demonstrate the excellent biocompatibility of the GN-ALG-DN hydrogels. This study highlights the design of robust shaped and structured supramolecular hydrogels from natural herb small molecules, which can serve as solid, edible, and stimuli-responsive active cargo delivery platforms for food, biomedical, and sustainable applications.
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Journal of Materials Chemistry B
·
2023
·
IF 7
Bin Zhu,Yu Liu,Yanlei Zhao,Xinyu Dou,Linbang Wang,Shuyuan Min,Xiaoguang Liu,Dong Qiu
The ideal skull defect repairing material should have good biocompatibility, mechanical properties, and contribute to osteogenesis. In this study, we designed and fabricated biodegradable, bioactive and mechanically robust porous scaffolds composed completely of biological materials. We used gelatin-chitosan blend as the matrix, sodium phytate instead of toxic glutaraldehyde for cross-linking, and the pH-neutral bioactive glass (PSC) to improve biological activity and mechanical properties. The chitosan-gelatin-30%PSC/sodium phytate composite scaffold avoided the problems of high toxicity in conventional cross-linking agents with glutaraldehyde, the poor mechanical support of pure chitosan or gelatin scaffold, and the mismatch of degradation rate with bone repair, being promising as a new candidate for skull defect repair.
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CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Min Wu,Zhou Xue,Caixia Wang,Tao Wang,Dongcheng Zou,Peng Lu,Xueping Song
Spoilage results in food waste and endangers consumer health, and the smart antibacterial packaging can effectively inhibit bacterial growth and reduce food spoilage . In this study, the smart antibacterial nanocellulose packaging films were developed by adding the pH-stimulated responsive microcapsules into cellulose nanofibril (CNF) film-forming. The microcapsules were synthesized by interfacial polymerization of Pickering emulsion . Carboxylated cellulose nanocrystals as solid particles stabilized the composited oil phase to prepare the oil-in-water Pickering emulsion. The emulsion with the particle concentration of 1.25 wt% and the oil phase mass fraction of 7.5 % processes excellent stability and uniform particle size, was chosen to synthesize microcapsules. The cinnamaldehyde in the film with the addition amount of microcapsules 0.6 g burst released in the first 1 h and then slowly, and the cumulative release at pH 2.0, 4.0, 5.5 and 7.2 was 28.43 μg/cm 2 , 18.84 μg/cm 2 , 16.52 μg/cm 2 and 12.89 μg/cm 2 , respectively. The inhibitory rate of film against both E. coli and L. monocytogenes reached 99 % at pH 4.0. The shelf life of pork packed by the film prolonged to nearly 9 d at room temperature . The developed films have the potential to be used in food packaging.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Wenxi Wang,Yiming Chen,Chongxin Xiao,Siying Xiao,Chuyi Wang,Qingling Nie,Peipei Xu,Jingbo Chen,Ruiyun You,Guifeng Zhang,Yudong Lu
Flexible wearable sensors can detect analytes continuously, in real time, and non-invasively, and their application in human health monitoring has received great attention. However, traditional sensors suffer from insufficient biocompatibility, wearing discomfort, and low detection sensitivity, so hydrogel is introduced as a sensor patch to improve the contact between skin and sensor, and combined with surface-enhanced Raman spectroscopy (SERS) technology for rapid and sensitive analysis of biomarkers in sweat. Here, a flexible SERS wearable sensor based on a sulfonated cellulose nanocomposite hydrogel (S-CNF-Ag NPs/PAA) was developed. The hydrogel was prepared by photo-crosslinking of sulfonated cellulose silver nanocomposites (S-CNF-Ag NPs) with acrylic acid (AA), which is a quick and easy preparation process. The network structure of hydrogel can retain small molecules and adsorb sweat through hydrophilic groups, which diffuse sweat into the hydrogel and can effectively collect the analyses in sweat. The introduction of cellulose and silver nanoparticles not only provides excellent mechanical and adhesive properties (toughness of ∼3790 kJ/m 3 , interfacial toughness of ∼116.23 J/m 2 ), but also good antimicrobial properties and biocompatibility. The SERS technology enabled the quantitative analysis of metabolites in sweat (the detection limits for urea and uric acid were 63.1 μM and 3.98 μM, respectively) and real-time monitoring of pH. S-CNF-Ag NPs/PAA sensor maintained excellent sensitivity, stability and mechanical properties during the detection process, effectively expanding the application of hydrogels in flexible SERS sensing and human health detection.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Fan Wang,Rongrong Ma,Jingling Zhu,Jinling Zhan,Jun Li,Yaoqi Tian
Steviol glycosides possess Bola-form amphiphilic structure, which can solubilize hydrophobic phytochemicals and exert physical modification to the hydrophilic matrix. However, the effect of steviol glycosides on the starch hydrogel is still unclear. Herein, the physicochemical properties, in vitro digestibility, and release behavior of starch hydrogel in the presence of steviol glycosides were investigated. The results showed that the addition of steviol glycosides promoted the gelatinization and gelation of starch, and endowed the starch hydrogel with softer texture, larger volume, and higher water holding capacity. The hydrophobic curcumin was well integrated into hydrogel by steviol glycosides, providing the gel with improved colour brilliance. The introduction of steviol glycosides hardly affected the digestibility of starch gel, but it promoted the release rate of curcumin. Notably, this release behavior was pH dependent, which tended to target the alkaline intestine. This work provided some theoretical supports for the development of sugar-free starchy foods.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Cong Yang,Wenjie Xu,Xin Meng,Xinlong Shi,Luhua Shao,Xiangliang Zeng,Zhenfei Yang,Sijian Li,Yutang Liu,Xinnian Xia
Giving the coating to exert a powerful active protective effect for metal substrates, such as self-healing property by encapsulating corrosion inhibitor into a pH-responsive release tool, is a crucial way to develop an efficient anticorrosive coating. Here, a pH-responsive hydrophilic controlled release system (BTA@ZIF-8@tannic acid, abbreviated ZBT) based on ZIF-8 for waterborne EP self-healing anticorrosive coating was reported. Encapsulation of BTA into ZIF-8 by a facile one-pot method and the resulting product showed a high loading percentage. The anticorrosion performance of composite coatings was studied by EIS, and the results indicated that ZBT could effectively enhance the protective performance of the coating and endow it with outstanding self-healing performance, in which the |Z| 0.01 Hz was about 2 orders of magnitude higher than that of pure EP coating after 20 days of immersion. The outstanding performance is related to the excellent compatibility of ZBT, the blocking effect of newly produced hydrophobic substances and the corrosion inhibitor and ferric tannate protective films formed on the exposed metal surface. In this work, tannic acid plays a role of killing two birds with one stone in enhancing the corrosion protection performance of the coating. This synergistic strategy opens a new possibility to fabricating excellent anticorrosive coatings with efficient self-healing functionality.
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JOURNAL OF FOOD SCIENCE
·
2021
·Vol. 86
·期 3
·677-686
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IF 3.167
Yuanyuan Chen,Yu Tang,Qiming Wang,Lin Lei,Jichun Zhao,Yuhao Zhang,Lin Li,Qiang Wang,Jian Ming
Absract The interaction between gluten and hydrocolloid additive, as well as the pH condition during dough formation is very important in making flour products. In this study, the influence of different pH conditions on the interactions between gluten proteins (including glutenin and gliadin) and carboxymethylcellulose (CMC), and on the rheological and microstructure changes of gluten proteins was investigated. The dynamic frequency sweep indicated CMC-gluten displayed more solid-like behavior under alkaline conditions than that under acidic conditions. The creep-recovery experiment suggested acidic conditions were not conducive to maintain the elasticity of CMC-gluten. Microstructural changes of various glutens with CMC showed that a higher ratio of β-sheets was observed in the CMC-gluten and CMC-glutenin under alkaline conditions. Total free sulfhydryl contents and changes in tryptophan microenvironment showed glutenin played a key role in the G polymerization with the addition of CMC. Lower surface hydrophobicity of CMC-gluten was displayed under acidic conditions. Scanning electron microscopy images showed that neutral and alkaline conditions were conducive to the network structure formation of CMC-gluten and CMC-glutenin. Practical Application This study investigated the interaction of CMC with gluten, gluten, and gliadin under different pH conditions, providing a basis for expanding dough quality improvement, and extending the in-depth application of CMC in the food industry.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Zhenpeng Li,Quanquan Lin,David Julian McClements,Yuying Fu,Hujun Xie,Teng Li,Guowen Chen
In this study, core-shell biopolymer nanoparticles were fabricated for the encapsulation and delivery of curcumin using a pH-driven method. The influences of the coating composition on the physicochemical properties and curcumin release characteristics of the core-shell nanoparticles were studied. Fourier transform infrared spectroscopy and X-ray diffraction analyses indicated that curcumin was encapsulated in an amorphous state inside the nanoparticles. Particle size and ζ-potential measurements indicated that the biopolymer nanoparticles were relatively stable under different environmental conditions: long term storage, heating, pH changes and salt. The DPPH radical scavenging activity of the curcumin was increased after encapsulation within the nanoparticles, whereas the gastrointestinal release of curcumin was prolonged. These results were attributed to the ability of alginate and NaCas to form a thick layer around the nanoparticles, which increased the steric and electrostatic repulsion between them, as well as inhibiting the release of curcumin.
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ACS Omega
·
2021
·
IF 3.512
Guodong Zheng,Jiahui Zheng,Le Xiao,Tongyi Shang,Yanjun Cai,Yuwei Li,Yiming Xu,Xiaoming Chen,Yun Liu,Bin Yang
In this study, a pH-responsive nano-prodrug was fabricated by conjugating emodin to the PEGylated polyethyleneimine (mPEG-PEI) with acid-sensitive boronate ester bonds. 1H NMR spectra results showed that emodin was effectively bonded to mPEG-PEI, and acid-sensitive assay further confirmed the formation of boronate ester bonds. The size and morphology of the nano-prodrug were ascertained through transmission electron microscopy (TEM) and dynamic light scattering (DLS), which showed that the prodrug has a sphere-like shape with hydrodynamic size around 102 nm at pH 7.4. Subsequently, a drug-release behavior assay was carried out to carefully investigate the acid-sensitive drug-delivery property of the prodrug. Moreover, in vitro cell viability assay confirmed the superior cytotoxic effect of the nano-prodrug against HeLa cells compared to free emodin. Furthermore, the antibacterial study showed that the nano-prodrug could inhibit the bacterial (both Gram-positive and Gram-negative) growth more effectively than free emodin. Overall, this study provides a promising paradigm of the multifunctional nano-prodrug for pH-responsive tumor therapy and antibacterial activity.
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Journal of Inorganic and Organometallic Polymers and Materials
·
2021
·Vol. 31
·期 5
·2054-2062
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IF 3.543
Huang Weihong,Si Haojie,Qing Yujie,Zhang Liming,Zhang Wenwen,Song Fei,Ni Xiaoni,Yang Wenming
A magnetic, core–shell structured pH-responsive molecularly imprinted polymer was prepared by surface imprinting technique and free radical polymerization for selective extraction of sulfamethoxazole. The imprinted polymer shell was prepared using 2-(Dimethylamino) ethyl methacrylate as pH-sensitive monomer, a certain amount of 4-vinylphenylbronic acid and methacrylic acid as common monomer to increase selectivity, sulfamethoxazole as template molecules. Excellent adsorption capacity (39.06 mg g −1 ) and selectivity (IF = 2.19) were achieved and the capture/release process can be regulated by pH value. In addition, it has been successfully applied to the detection of sulfamethoxazole in water samples and the recovery rate reached 96.2%. This study provides a new method and idea for the selective separation and detection of sulfamethoxazole in actual samples.
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ACS Omega
·
2021
·
IF 3.512
Yinghua Tao,Dan Zheng,Jingyang Zhao,Kefeng Liu,Jing Liu,Jiandu Lei,Luying Wang
Pharmaceutical science based on biological nanotechnology is developing rapidly in parallel with the development of nanomaterials and nanotechnology in general. Pectin is a natural polysaccharide obtainable from a wide range of sources. Here, we show that doxorubicin (DOX)-conjugated hydrophilic pectin (PET) comprising an amphiphilic polymer loaded with hydrophobic dihydroartemisinin (DHA) self-assemble into nanoparticles. Importantly, conjugated DOX and DHA could be released quickly in a weakly acidic environment by cleavage of the acid-sensitive acyl hydrazone bond. Confocal microscopy and flow cytometry confirmed that these PET-DOX/DHA nanoparticles efficiently delivered DOX into the nuclei of MCF-7 cells. Significant tumor growth reduction was monitored in a female C57BL/6 mouse model, showing that the PET-DOX/DHA nanoparticle-mediated drug delivery system inhibited tumor growth and may improve therapy. Thus, we have demonstrated that pectin may be useful in the design of materials for biomedical applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Hongbo Lu,Chunli Wang,Xueming Liu,Jing Zhang,Zhang Lin,Zhengping Hao,Gang Pan
Arsenic sulfide sludge (ASS) is a typical precipitation product of acid smelting wastewater. Previous study reported that when exposed to sunlight, the release and oxidation of As(III) in ASS were markedly accelerated. However, the key factor to trigger the photocatalytic transformation of ASS is still unclear. Herein, we revealed that the coexisting Fe(II)/Fe(III) ions were critical to promote the photo-oxidation of released As(III) under visible light. We further validated that Fe(II)-stimulated photo-oxidation mechanism of As(III) in ASS was pH-dependent. In acid conditions, OH and SO 4 − were promoted by Fe(II)/Fe(III) cycling catalysis with the assistance of the reductive sulfur species from ASS, e.g. S 2− and SO 3 2− , and thus accelerated the oxidation of As(III). While in neutral conditions, the nascent ferric hydroxide colloids enhanced the oxidation rate of As(III) via photo-induced ligand-to-metal-charge transfer (LMCT) mechanism. These findings help in predicting and controlling the fate of real arsenic-containing sludge in sunlit environments.
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