Nanoscale
·
2019
·Vol. 11
·期 19
·9457-9467
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IF 6.97
Xunan Jing,Zhe Zhi,Liming Jin,Fei Wang,Youshen Wu,Daquan Wang,Kai Yan,Yongping Shao,Lingjie Meng
Multifunctional nanodrugs with the integration of precise diagnostic and effective therapeutic functions have shown great promise in improving the efficacy of cancer therapy. We report herein a simple and effective approach to directly assemble an anticancer drug (curcumin), a photodynamic agent (Ce6) and tumor environment-sensitive molecules into cross-linked polyphosphazene and coat on superparamagnetic Fe3O4 nanoclusters to form discrete nanoparticles (termed as FHCPCe NPs). FHCPCe NPs have high physiological stability and good biocompatibility, and can enhance accumulation in tumor tissue via the enhanced permeability and retention effect. Meanwhile, the FHCPCe NPs exhibit an effective performance of dual-modality magnetic resonance imaging (MRI) due to the Fe3O4 cores and fluorescence imaging (FL) in the xenografted HeLa tumor because of the fluorescence of Ce6. Importantly, under the conditions of supernormal glutathione levels and acidic microenvironment in tumor tissue, curcumin and Ce6 can be effectively released by the degradation of FHCPCe NPs. Therefore, excellent anti-tumor effects both in vitro and in vivo have been achieved by synergistic chemotherapy/photodynamic therapy (CT/PDT) using multifunctional NPs. Our study highlights the promise of developing multifunctional nanomaterials for accurate multimodal imaging-guided highly sensitive therapy of cancer.
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Journal of Physical Chemistry C
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2019
·
IF 4.309
Kecheng Hu,Jun Tang,Shixiong Cao,Qi Zhang,Jianli Wang,Zhibin Ye
We report in this paper the design and synthesis of a pH-responsive polymeric interfacial catalyst (PIC) via one-step grafting of 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) onto a polyaryletherketone having pendant benzimidazole groups (SCBI-PAEK-6F). The TEMPO-functionalized polymer has been systematically characterized with 1H nuclear magnetic resonance, Fourier-transform infrared spectroscopy, elemental analysis, contact angle, and transmission electron microscopy. Moreover, this well-designed polymer has been applied in the oxidation of alcohols under Montanari conditions. It is found that the functionalized polymer can aggregate at the water–oil interface and act as an efficient stabilizer to facilitate the formation of a stable Pickering emulsion, which shows outstanding catalytic activity for alcohol oxidation through the microreactor mechanism. Moreover, the PIC is featured with desirable high pH responsiveness due to the valuable benzimidazole groups. De-emulsification of the Pickering emulsion reaction system can be conveniently triggered by simply tuning the system pH value to 3, thus facilitating the facile recovery of the PIC. In addition, the sustainable catalyst can be reused for subsequent cycles of alcohol oxidation without appreciable loss in catalytic activity or selectivity.
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CERAMICS INTERNATIONAL
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2019
·
IF 3.45
Keping Zhang,Chengqiang Ding,Xiaolin Liu,Jun Gao,Datong Wu,Yong Qin,Yong Kong
Tubular mesoporous silica (T-mSiO 2 ) was facilely synthesized through a co-template method by using cetyltrimethylammonium bromide and α-Fe 2 O 3 as the dual templates, and then disulfide (–SS–) bonds and carboxyl groups (–COOH) were introduced to the resultant T-mSiO 2 via the reaction with 2-carboxyethyl 2-pyridyl disulphide. The obtained –SS– grafted T-mSiO 2 (SS-T-mSiO 2 ) was then grafted with chitosan (CS) via the amidation reaction between the –COOH groups on SS-T-mSiO 2 and the –NH 2 groups on CS. The CS grafted SS-T-mSiO 2 (CS-SS-T-mSiO 2 ) was fully characterized by various technologies such as transmission electron microscopy , energy dispersive X-ray spectroscopy and Fourier transform infrared spectroscopy . Finally, the as-synthesized CS-SS-T-mSiO 2 was used as the carrier for redox and pH dual-triggered delivery of 5-fluorouracil (5-FU), an anti-cancer drug, and the results indicate that the developed CS-SS-T-mSiO 2 might be a potential responsive carrier for redox and pH dual-triggered drug delivery.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Tao Li,Shaoyu Lü,Jia Yan,Xiao Bai,Chunmei Gao,Mingzhu Liu
Layer-by-layer (LBL) self-assembly based on natural polysaccharides is drawing significant attention in various applications. However, its application in fertilizers is limited. In this study, LBL electrostatic self-assembly technology was employed to prepare an environment-responsive fertilizer with natural polyelectrolyte layers of chitosan and lignosulfonate deposited on polydopamine-coated ammonium zinc phosphate. The morphology of the fertilizer was evaluated by scanning electron microscopy, transmission electron microscopy, and atomic force microscopy. The composition and self-assembly process of the fertilizer were characterized by elemental analysis, Fourier transform infrared spectroscopy, UV–vis absorption spectroscopy, zeta potential analysis, thermal analysis, X-ray photoelectron spectroscopy, and inductively coupled plasma atomic emission spectroscopy. Excellent pH-responsive behavior was observed by the nutrient release results. In an alkaline medium at room temperature, the nutrient release rate can be clearly accelerated compared with that in acidic and neutral media. Moreover, pot experiments showed that the fertilizer can effectively promote plant growth. The pH-responsive environment-friendly fertilizer can control nutrient release and avoid excessive release of nutrients, showing promising applications in modern green and sustainable agriculture and horticulture.
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CARBOHYDRATE POLYMERS
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2019
·
IF 6.044
Guanghui Hou,Junmin Qian,Weijun Xu,Tiantian Sun,Yaping Wang,Jinlei Wang,Lijie Ji,Aili Suo
Chemo-photothermal combination therapy is a promising strategy for cancer treatment. In this study, to achieve the combined photothermal-chemotherapy of breast cancer, a pH-sensitive oxidized hyaluronic acid-decorated dihydroxyphenyl/hydrazide bifunctionalized hydroxyethyl chitosan (DHHC)-gold nanorod (GNR) conjugate was developed. DHHC was synthesized by successive dihydroxyphenylation and hydrazidation of hydroxyethyl chitosan through carbodiimide reaction and click chemistry, respectively. The conjugate was obtained by chemically bonding DHHC onto GNR via Au-catechol bonds. Doxorubicin (DOX) was loaded onto the conjugate via an acid-labile hydrazone linkage with a drug loading content of 5.1%. DOX-loaded conjugate displayed good stability in neutral aqueous solutions and exhibited pH-responsive drug release and surface charge reversal behaviors. In vitro biological studies indicated that the conjugate could be effectively internalized by breast cancer MCF-7 cells and synergistic therapeutic effects were demonstrated, suggesting its great potential in combined photothermal-chemotherapy of breast cancer.
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IET Nanobiotechnology
·
2019
·Vol. 13
·期 6
·640-649
·
IF 1.925
Wanxia Wang,Youyun Wang,Yu Wang,Huameng Gong,Hongda Zhu,Mingxing Liu
New drug delivery system (ZnO@CMS) of the redox and pH dual-stimuli responsive based on colloidal mesoporous silica nanoparticles (CMS) has been designed, in which zinc oxide quantum dots (ZnO QDs) as a capping agent was conjugated on the surface of nanoparticles by amide bonds. The release behaviour of doxorubicin (DOX) as the model drug from ZnO@CMS (ZnO@CMS-DOX) indicated the redox and pH dual-stimuli responsive properties due to the acidic dissolution of ZnO QDs and cleavage of the disulphide bonds. The haemolysis and bovine serum albumin adsorption assays showed that the modification of ZnO QDs on the mesoporous silica nanoparticles modified by mercapto groups (CMS-SH)(ZnO@CMS) had better biocompatibility compared to CMS-SH. The cell viability and cellular uptake tests revealed that the ZnO@CMS might achieve the antitumour effect on cancer cells due to the cytotoxicity of ZnO QDs. Therefore, ZnO@CMS might be potential nanocarriers of the drug delivery system in cancer therapy. The in vivo evaluation of ZnO@CMS would be carried out in future work.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2019
·
IF 4.784
Xiaoxiao Sun,Chao Liu,A.M. Omer,Wuhuan Lu,Shuxing Zhang,Xun Jiang,Hongjie Wu,Di Yu,Xiao-kun Ouyang
To develop relatively green and ecofriendly smart vehicles for colon-specific drug delivery, carboxymethyl cellulose (CMC) and chitosan (CS) pH-sensitive biopolymers were used in this study. To overcome the weaknesses of CMC carriers, such as poor mechanical performance and an explosive drug release, zinc oxide (ZnO) nanoparticles were incorporated into CMC beads and then coated with a CS layer via a self-assembly technique to form core–shell polyelectrolyte complexes. An anticancer drug, 5-fluorouracil (5-FU), used as a model drug, was loaded into ZnO/CMC/CS bio-nanocomposite beads. Fourier transform infrared spectroscopy , scanning and transmission electron microscopy , and thermogravimetric analysis were used to characterize the chemical structure, morphological changes, and thermal properties of the developed drug carrier, respectively. By studying their swelling and in vitro 5-FU release profiles under simulated gastrointestinal conditions, the pH sensitivity of the developed bio-nanocomposite hydrogel beads could be investigated. The obtained beads with reduced porosity could effectively encapsulate 5-FU and showed self-sustained release behavior depending on the concentrations of CMC, CS, and ZnO nanoparticles. The developed beads also demonstrated a capacity for biodegradation. The results indicated that the ZnO/CMC/CS bio-nanocomposite beads exhibited pH-sensitivity and could be applied efficiently as biodegradable carriers for colon-specific 5-FU delivery.
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JOURNAL OF POLYMER SCIENCE PART B-POLYMER PHYSICS
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2018
·Vol. 56
·期 24
·1636-1644
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IF 2.499
Yixia Li,Jianhao Si,Haiyan Fan,Xiaodong Ye
The micelles formed by reduction-sensitive amphiphilic copolymer have emerged as promising drug nanocarriers due to the controlled drug release and effective anticancer activity triggered by the reducing stimulation. However, the effect of pH on the stability and guest exchange of the micelles formed by reduction-sensitive copolymer have not been systemically investigated. Herein, the micelles formed by a reduction-sensitive copolymer poly(ε-caprolactone)- b -poly[oligo(ethylene glycol) methyl ether methacrylate] (PCL–SS–POEGA) with a single disulfide group at different pH values loaded with dyes 3,3′-dioctadecyloxacarbocyanine perchlorate/1,1′-dioctadecyl-3,3,3′,3′-tetramethylindocarbocyanine perchlorate (DiO/DiI) were prepared through the precipitation-dialysis method. In addition, mixed micelles formed by different contents of reduction-sensitive and reduction-insensitive copolymers encapsulated with DiO/DiI at pH 7.5 were also prepared by the similar approach. The effects of pH and the content of reduction-sensitive copolymer on guest exchange of these micelles were studied by the fluorescence resonance energy transfer method. Results show that the pH value in the environment has great influence on the guest exchange rate of reduction-sensitive micelles in the presence of 10 mM dithiothreitol (DTT) and slight effect on that in the absence of DTT. Under a reducing environment, the guest exchange rate of the micelles containing various contents of disulfide-linked copolymer increases with the increasing content of PCL–SS–POEGA. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2018 , 56 , 1636–1644
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2019
·Vol. 220
·期 15
·1900187
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IF 2.622
Haipeng Luo,Yonghui Lin,Qiuju Tang,Wei Hu,Yaping Wang,Zhentao Lei,Zaizai Tong
Regulation of crystalline micelles is difficult to achieve because of the strong solidification of crystallization. In this present work, an amphiphilic triblock copolymer poly(ethylene oxide)- b -poly(ε-caprolactone)- b -poly(4-vinylpyridine) (PEO- b -PCL- b -P4VP) is prepared, in which the P4VP block serves as an H-bonding acceptor. It is originally self-assembled into crystalline lamellar micelles in aqueous solution. Subsequently, the effect of varying pH and organic diacids on morphological transition is investigated in detail. Lamellae-to-cylinder-to-sphere transitions are observed after decreasing the pH or with the addition of organic diacids with different chain spacers. The decreasing pH causes increasing hydrophilicity of the P4VP block, while adding organic diacids results in an increasing corona swelling of the P4VP segment, both of which lead to a decreasing crystallinity of the poly(ε-caprolactone) core. Consequently, morphological variety changing from lamellar to worm-like to spherical micelles can be achieved.
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CHEMISTRY-A EUROPEAN JOURNAL
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2019
·Vol. 25
·期 35
·8353-8362
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IF 5.16
Jiamei Han,Guohai Liang,Da Xing
Graphical Zwitterions pass the acid test : A zwitterionic iron complex that can dissociate rapidly in weakly acidic environment was shown to serve as a positive contrast agent for tumor-specific magnetic resonance imaging (see figure). Accurate diagnosis of tumor characteristics, including its location and boundary, is of immense value to subsequent therapy. Activatable magnetic resonance imaging (MRI) contrast agents that respond to tumor-specific microenvironments, such as the redox state, pH, and enzyme activity, enable better mapping of tumor tissue. However, the practical application of most reported activatable agents is hampered by problems including potential toxicity, inefficient elimination, and slow activation. In this study, we developed a zwitterionic iron complex (Fe-ZDS) as a positive MRI contrast agent for tumor-specific imaging. Fe-ZDS could dissociate in weakly acidic solution rapidly, accompanied by clear longitudinal relaxivity ( r 1 ) enhancement, which enabled the complex to act as a pH-sensitive contrast agent for tumor-specific MR imaging. In vivo experiments showed that Fe-ZDS rapidly enhanced the tumor-to-normal contrast ratio by >40 %, which assisted in distinguishing the tumor boundary. Furthermore, Fe-ZDS circulated freely in the bloodstream and was excreted relatively safely via kidneys owing to its zwitterionic nature. Therefore, Fe-ZDS is an ideal candidate for a tumor-specific MRI contrast agent and holds considerable potential for clinical translation.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2019
·
IF 4.784
Xiaoxiao Sun,Chao Liu,A.M. Omer,Li-Ye Yang,Xiao-kun Ouyang
A new pH-sensitive drug carrier based on alginate (Alg), chitosan (Cs), and kappa-carrageenan (kC) marine biopolymers was developed, comprising a dual-layered polyelectrolyte complexes microbead structure. Fourier-transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), and scanning electron microscopy (SEM) were used to investigate the structures, thermal stability , and morphological changes, respectively, of the microcapsules we developed. In the intestinal environment (pH 7.4), the stability and swelling of Alg microbeads were enhanced after generation of the dual-layered polyelectrolyte complexes. The in vitro release profiles of 5-fluorouracil under simulated GI conditions were also examined. At gastric pH (1.2), the cumulative 5-FU release percentage was decreased by introduction of the additional kC layer from 14% in Alg/Cs microbeads to 7% in the dual-layered Alg/Cs/kC microbeads. Additionally, the release profiles were greatly improved under simulated intestinal and colon conditions. Finally, the microbeads were all biodegradable and showed no cytotoxicity in Chang liver cells. Our results clearly indicate that the dual-layer pH-sensitive Alg/Cs/kC microbeads could be used effectively for the targeted delivery of anticancer drugs to the colon.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2018
·Vol. 165
·期 3
·C145
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IF 3.662
Xuehui Liu,Chuanjun Gu,Zheng Ma,Xiumin Ma,Baorong Hou
In this study, TiO2 containers with an empty core and a mesoporous shell were successfully synthesized via hydrothermal reaction. The as-prepared TiO2 was used as carrier to load the corrosion inhibitor 2-mercaptobenzimidazole (MBI). The outer shell of inhibitor-loaded containers was modified by a SiO2 film, which was obtained from hydrolysis of tetraethyl orthosilicate (TEOS) and (3-aminopropyl) triethoxysilane (APTES). The structure of the TiO2 containers was studied using X-ray diffraction (XRD) analysis, field emission scanning electron microscopy (FESEM), and Fourier transform infrared (FTIR) spectrometry. The release behavior of the corrosion inhibitor was investigated using UV-visible spectroscopy. The corrosion protection performance of the water-based epoxy coating with modified TiO2 containers was studied by using electrochemical impedance spectroscopy (EIS) and a scanning Kelvin probe (SKP). The coating with modified TiO2 containers demonstrated enhanced film barrier properties compared with blank coating. Results obtained from SKP measurements confirmed active corrosion protection performance of the studied TiO2 containers.
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