EUROPEAN POLYMER JOURNAL
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2019
·
IF 3.621
Jie Wu,Ximing Tian,Yihua Yin,Meng He,Weiquan Cai,Guanghua He,Wenjin Xu,Yue Dai,Jiahao Mai,Mengqi Gan,Fengxinjia Zhang
To improve hydrolytic stability and biological half-life and anticancer efficacy of the anti-cancer drug melphalan (Mel), a novel esterification strategy was developed to fabricate a pH/enzyme dual-responsive polymer prodrug (mPEG-Mel) via the formation of an ion bond between the carboxyl group in Mel and diazotized p-aminobenzoate-terminated poly(ethylene glycol) monomethyl ether (mPEG-N 2 + ) followed by light-induced conversion of the ionic bond to an ester bond. The prodrug could self-assemble into nanoparticles. Under physiological conditions (pH 7.4), the nanoparticles exhibited a regular core-shell structure with about 100 nm, which could effectively inhibit the hydrolysis of pharmacophores in Mel structure and showed the long-circulation ability. While pH dropped to 5.0, an obvious increase in the nanoparticle size was observed and enhanced by different concentrations of cathepsin B (CTB), reaching a diameter of 675 nm or more in the presence of 2.0 µg/mL CTB. The nanoparticles showed minimal drug release at pH 7.4 (less than 10% in 24 h); however, drug release could be significantly accelerated in a CTB-containing medium at pH 5.0. Cell experiments showed that the half-inhibitory concentration (IC50) of nanoparticles was 1.00 µg/mL, which was about 5 times lower than that of free Mel (5.00 µg/mL), and indicating that the nanoparticles were more cytotoxic to cancer cells (4T1 cells). However, significantly reduced cytostatic effects were observed for normal cells (3T3 cells). In addition, cell uptake observation further supported the above experimental results, a stronger red fluorescence in 4T1 cells was observed for NR-loaded nanoparticles, which meant that the nanoparticles could release drug in response to pH/enzyme stimulation. Thus, mPEG-Mel based pH/enzyme double-response polymer prodrug nanoparticles could effectively enhance drug stability and anticancer efficacy.
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Materials Science & Engineering C-Materials for Biological Applications
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2020
·
IF 5.88
Guoping Li,Mingliang Pei,Peng Liu
Carbon quantum dots (CQDs) show promising potential for tumor imaging owing to their unique superior fluorescent properties. However, the small particle size limits their practical application. Here, pH/reduction dual-responsive comet-shaped PEGylated CQD-DOX conjugate prodrug, DOX-Hy-CQD-SS-PEG with DOX content of 28.5%, was designed with the hydrophobic acid-labile DOX conjugated CQDs as comet nucleus and the few hydrophilic bioreducible detachable PEG brushes as comet tails. The comet-shaped DOX-Hy-CQD-SS-PEG prodrug could self-assemble into unique micelles with mean diameter of 127 nm. The DOX-Hy-CQD-SS-PEG micelles possessed excellent pH/reduction dual-responsive drug release with low drug leakage of 9% in 150 h. Furthermore, the fluorescent CQDs was recovered after DOX release and de-PEGylation, demonstrating their potential application for real-time response of therapy.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Qiang Zeng,Yongji Huang,Leiming Huang,Liang Hu,Daoling Xiong,Hui Zhong,Zhiguo He
The reduction of Cr(VI) by iron-based materials was inhibited under neutral and alkaline conditions due to the production of precipitates. In this work, a novel composite with a wide pH range application in the remediation of Cr(VI) contamination, SiO 2 /nano-FeC 2 O 4 composite (SNFC), was prepared from natural biotite-containing minerals. Transmission electron microscope (TEM) analysis indicated that nano-FeC 2 O 4 with average particle size of 10.08 nm was uniformly coated on the surface of layered minerals. Batch experiments results showed that Cr(VI) was completely removed in the pH range of 2–10 within 60 min at an initial Cr(VI) concentration of 20 mg/L. The removal rate of Cr(VI) was decreased when the initial pH value increased from 2 to 6 and then kept at constant when the initial pH value increased from 6 to 10. Furthermore, continuous fixed bed column studies showed that simulated permeable reactive barriers (PRB) with SNFC was considerably effective for in situ removal of Cr(VI) from groundwater under alkaline conditions. Characterizations of X-ray diffraction (XRD) and scanning electron microscope (SEM) suggested that the reactive component in the composite for Cr(VI) removal was nano-FeC 2 O 4 rather than biotite itself. The Cr(VI) removal mechanisms of SNFC involved reduction, precipitation and surface complexation. These results plus the preliminary cost analysis indicated that the composite was an efficient, economical, and easy for mass production material with application for remediation of Cr(VI) polluted groundwater in a wide pH range.
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JOURNAL OF SURFACTANTS AND DETERGENTS
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2019
·Vol. 23
·期 1
·169-176
·
IF 1.672
Jian Zou,Yigang Liu,Qiuxia Wang,Hao Liu,Han Jia,Peng Lian
The dynamic noncovalent interaction between the anionic surfactant sodium dodecyl benzene sulfonate (SDBS) and 1,3-diphenylguanidine (DPG) was employed to control the interfacial activity of the surfactant. At high HCl concentration (1000 mg L −1 ), the SDBS/DPG n+ system could reduce the water/oil interfacial tension (IFT) to 10 −4 mN m −1 order of magnitude, which was much lower than the IFT values in the SDBS/DPG + system with a low HCl concentration (100 mg L −1 ) and the individual SDBS system by three and four orders of magnitude, respectively. The pH-switchable protonation of amido groups in DPG molecules determines the SDBS/DPG molecular interaction and the amplitude of IFT reduction, which was confirmed by control experiments using two other surfactants (sodium dodecyl sulfate [SDS] and dodecyl trimethylammonium bromide [DTAB]). Moreover, the investigation of the NaCl and temperature effects on the IFT indicated the intensity of mixed SDBS/DPG n+ adsorption layers at the water/oil interface.
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ACS Applied Materials & Interfaces
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2018
·
IF 8.097
Liyan Bi,Yunqing Wang,Ying Yang,Yuling Li,Shanshan Mo,Qingyin Zheng,Lingxin Chen
Conventional research on surface-enhanced Raman scattering (SERS)-based pH sensors often depends on nanoparticle aggregation, whereas the variability in nanoparticle aggregation gives rise to poor repeatability in the SERS signal. Herein, we fabricated a gold nanorod array platform via an efficient evaporative self-assembly method. The platform exhibits great SERS sensitivity with an enhancement factor of 5.6 × 107 and maintains excellent recyclability and reproducibility with relative standard deviation (RSD) values of less than 8%. On the basis of the platform, we developed a highly sensitive bovine serum albumin (BSA)-coated 4-mercaptopyridine (4-MPy)-linked (BMP) SERS-based pH sensor to report pH ranging from pH 3.0 to pH 8.0. The intensity ratio variation of 1004 and 1096 cm–1 in 4-MPy showed excellent pH sensitivity, which decreased as the surrounding pH increased. Furthermore, this BMP SERS-based pH sensor was employed to measure the pH value in C57BL/6 mouse blood. We have demonstrated that the pH sensor has great advantages such as good stability, reliability, and accuracy, which could be extended for the design of point-of-care devices.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2018
·
IF 4.229
Baodong Mao,Bo Wang,Furong Yu,Kewei Zhang,Zhengyuan Zhang,Jinhui Hao,Junbo Zhong,Yanhong Liu,Weidong Shi
In this paper, a facile hydrothermal synthetic strategy was developed for MoS 2 nanoflowers with enlarged interlayer spacing on the carbon cloth (CC) as a high efficiency cathode electrode for hydrogen evolution reaction (HER) under wide pH condition . It was observed that the loading amount of MoS 2 has a major impact on the HER performance, where the optimized MoS 2 /CC exhibited a low onset potential of 94 mV and a small Tafel slope of 50 mV dec −1 in strong acid solution (pH = 0). The improved HER performance can be contributed to the enlarged interlayer spacing, abundant defects and more exposed active sites in the small size MoS 2 nanosheets as revealed by XRD and HRTEM. Meanwhile, it also exhibited relatively good performance for HER under basic and neutral conditions with the overpotentials of 188 (pH = 14) and 230 (pH = 7) mV to achieve current density of 10 mA cm −2 and the Tafel slopes of 52 and 84 mV dec −1 , respectively.
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CHEMICAL ENGINEERING JOURNAL
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2018
·
IF 6.735
Shaolong Yang,Zhitao Han,Xinxiang Pan,Bojun Liu,Dongsheng Zhao
UV/chlorine has attracted much attention in flue gas and water treatment fields in recent years. However, only a few studies highlighted gas pollutants removal performance of UV/chlorine method in real water. In this study, nitrogen oxide (NO x ) removal using UV-irradiated electrolyzed seawater (UV/electrolyzed seawater) was explored under simulated seawater environment in a semi-batch photochemical reactor. Comparison experiments between UV/H 2 O 2 and UV/chlorine in both freshwater and seawater systems were performed. Results showed that NO removal efficiency in UV/chlorine freshwater system was higher than those in UV/chlorine seawater system, due to radical scavenging effects of water matrices in seawater. Several strong reactive radicals (e.g., OH, Cl, OCl, ClOH − ) yielded from UV/chlorine system were considered to contribute to NO x removal, among which the role of OH radical was confirmed by radical-trapping experiments. The alkalinity of the seawater adversely impacted contributions of these reactive radicals to NO x removal, which caused a sharp drop in NO x removal efficiencies. Comparatively, the chloride ion in seawater had slight influences on NO x removal efficiencies of UV/electrolyzed seawater. Then, optimization of NO x removal efficiencies against three key variables (active chlorine concentration, UV irradiation dose, and initial pH) was investigated in simulated seawater using Design Expert Software. A regression model of NO x removal efficiency was obtained with satisfactory accuracy. Results indicated that active chlorine concentration and UV irradiation dose significantly influenced NO x removal efficiencies, compared with pH effects. Furthermore, NO x removal mechanisms involved in reactive radicals were discussed for UV/electrolyzed seawater method. Due to pH-dependent characteristics of both active chlorine species and carbonate species in electrolyzed seawater, NO x removal pathways by UV/electrolyzed seawater were different as the environment changed from acid to alkalinity.
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ADVANCED FUNCTIONAL MATERIALS
·
2018
·Vol. 28
·期 23
·1800011
·
IF 13.325
Zhiyong Song,Yang Wu,Qi Cao,Huajuan Wang,Xiangru Wang,Heyou Han
To satisfy the ever-growing demand in bacterial infection therapy and other fields of science, great effort is being devoted to the development of methods to precisely control drug release and achieve targeted use of an active substance at the right time and place. Here, a new strategy for bacterial infection combination therapy based on the light-responsive zeolitic imidazolate framework (ZIF) is reported. A pH-jump reagent is modified into the porous structure of ZIF nanoparticles as a gatekeeper, allowing the UV-light (365 nm) responsive in situ production of acid, which subsequently induces pH-dependent degradation of ZIF and promotes the release of the antibiotic loaded in the mesopores. The combination of the UV-light, the pH-triggered precise antibiotic release, and the zinc ions enables the light-activated nanocomposite to significantly inhibit bacteria-induced wound infection and accelerate wound healing, indicating a switchable and synergistic antibacterial effect. The light irradiated accumulation of acid ensures the controlled release of antibiotic and controlled degradation of ZIF, suggesting the therapeutic potential of the metal–organic frameworks-based smart platform for controlling bacterial infection.
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INORGANIC CHEMISTRY
·
2018
·
IF 4.7
He-Qi Zheng,Chun-Yan Liu,Xue-Yu Zeng,Jin Chen,Jian Lü,Rong-Guang Lin,Rong Cao,Zu-Jin Lin,Jin-Wei Su
Natural enzyme mimetics with high catalytic activity at nearly neutral pH values are highly desired for their applications in biological systems. Herein for the first time a stable MOF, namely MOF-808, has been shown to possess high intrinsic peroxidase-like catalytic activity under acidic, neutral, and alkaline conditions. As a novel peroxidase mimetic, MOF-808 can effectively catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine when H2O2 serves as oxidant, accompanied by a significant color variation in the solution. The catalytic activity and the color variation were greatly dependent on H2O2 concentration, and thus MOF-808 can be applied to the colorimetric sensing of H2O2. The H2O2 detection limit is 4.5 μM, and the linear range is 10 μM to 15 mM. In view of the significant inhibition effect produced by ascorbic acid, a facile and sensitive approach for colorimetric sensing of ascorbic acid was successfully established. The AA detection limit is 15 μM, and the linear range is 30–1030 μM. Further investigation found that the catalytic activity of MOF-808 could be mainly ascribed to the Zr–OH(OH2) groups. Such active Zr–OH(OH2) groups can be effectively shielded by gluconic acid, and subsequently the catalytic activity of MOF-808 was significantly suppressed. With these findings, a facile and selective colorimetric assay for glucose sensing has been successfully explored via combination of the glucose oxidation with the TMB oxidation. The glucose detection limit is 5.7 μM, and the linear range is 5.7–1700 μM. MOF-808 is one of the best colorimetric biosensors among the peroxidase mimics reported for H2O2, AA, and glucose detection.
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Nanoscale
·
2018
·Vol. 11
·期 9
·3814-3826
·
IF 7.233
Mingmao Chen,Feifei Song,Yan Liu,Jia Tian,Chun Liu,Ruyue Li,Qiqing Zhang
In cancer therapy, chemotherapeutic drugs frequently encounter multidrug resistance (MDR) induced by the overexpression of drug transporters such as P-glycoprotein (P-gp). Herein, in order to overcome MDR and improve the effectiveness of chemotherapy, we developed a novel pH-sensitive charge-reversal and NO generation liposomal system by modifying a pH-sensitive polymer (PEG-PLL-DMA) on the surface of cationic liposomes for delivering a NO donor (DETA NONOate) and a chemotherapy drug (paclitaxel, PTX) into MDR cells. The proposed liposomal system (PTX/NO/DMA-L) exhibited a distinctive charge-reversal capacity, which was negatively charged under physiological conditions (pH 7.4) but could reverse to positive charge in a tumor microenvironment (pH 6.5) due to the cleavable amide linkages formed between PEG-PLL and DMA, leading to the improvement of cell uptake. Once arrived in the endosomes and lysosomes (pH 5.0), DETA NONOate was triggered to decompose and release NO, which further promoted the quick release of PTX and inhibited the P-gp mediated efflux. The charge-reversal, NO generation and NO-triggered rapid release of drugs could significantly increase the accumulation of PTX in tumors and eventually improve the antitumor efficacy. These results indicate that this dual pH-sensitive liposomal system is a highly promising approach for chemotherapy and may pave a new avenue for overcoming MDR in cancer.
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FEBS LETTERS
·
2018
·Vol. 593
·期 2
·175-186
·
IF 2.999
Shengnan Yang,Yuan Zhang,Fukui Shen,Xiaoyao Ma,Man Zhang,Yuanyuan Hou,Gang Bai
Baicalin is one of the main flavonoids of the dried root of Scutellaria baicalensis Georgi and is reported to exert beneficial effects on the regulation of glucose/lipid metabolism. However, understanding its specific target and unique mechanism for improving glucose utilization is a challenge. In this paper, target fishing with a baicalin probe reveals that baicalin interacts with AKT. An immunofluorescence assay further demonstrates the colocalization of baicalin with AKT in the cytoplasm. A competitive test and virtual docking show that baicalin might bind to the pleckstrin homology domain of AKT. This specific binding hampers AKT membrane translocation, activates the phosphorylation of AKT on Ser473, induces the downstream glycogen synthase kinase 3β activation, and affects glycogen synthesis.
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Acta Pharmaceutica Sinica B
·
2018
·
IF 6.014
Shuzhen Ren,Mingyu Liu,Chao Hong,Guowen Li,Jiabin Sun,Jianying Wang,Lei Zhang,Yan Xie
Pharmaceutical cocrystals are a promising technology that can be used to improve the solubility of poor aqueous compounds. The objective of this study was to systematically investigate the solubility of myricetin (MYR) cocrystals, including their kinetic solubility, thermodynamic solubility, and intrinsic dissolution rate (IDR). The effects of pH, surfactant, ion concentration, and coformers on the cocrystal solubility were evaluated. Furthermore, single crystal structures of MYR, myricetin–isonicotinamide (MYR–INM) and myricetin–caffeine (MYR–CAF) cocrystals were analyzed to discuss the possible reasons for the enhancement of cocrystal solubility from the perspective of the spatial structure. The results indicated that the kinetic solubility of MYR cocrystals was modulated by pH and cocrystal coformer (CCF) ionization in buffer solution, while it primarily depended on the CCF solubility in pure water. In addition, the solubility of MYR cocrystals was increased in a concentration dependent fashion by the surfactant or ion concentration. The thermodynamic solubility of MYR–INM (1:3) cocrystals decreased with the increases of the pH value of the dissolution media. The IDR of MYR cocrystals was faster than that of MYR in the same medium and extremely fast in pH 4.5 buffer. The improved solubility of MYR cocrystals was probably related to the alternate arrangements of MYR and INM/CAF molecules and increased intermolecular distance. The present study provides some references to investigate the solubility behavior of pharmaceutical cocrystals.
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