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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ACS Applied Materials & Interfaces
·
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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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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TALANTA
·
2019
·
IF 4.916
Yang Xing,Ying Zhou,Li Fan,Yajuan Yang,Yuan Zhang,Xu Deng,Chuan Dong,Shaomin Shuang
Herein, we figured out a novel ratiometric fluorescent probe based on Janus silica nanoparticles (SiO 2 NPs) where fluorescein isothiocyanate (FITC) and rhodamine B (RB) were asymmetrically functionalized for intracellular pH detection. With this unique strategy, the probe exhibited dual emission bands at 530 and 580 nm upon excitation at a single wavelength of 488 nm. The pH titrations of the probe showed a remarkable increase in ratiometric intensities ratio (I 530nm /I 580nm ) when the pH was switched from 3.0 to 8.0 with a acid dissociation constant (pKa) value of 6.64. The probe was successfully applied to imaging and detection of pH in living cells without noticeable cytotoxicity, indicating that it is a promising candidate for bioanalysis and bioimaging.
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JOURNAL OF SURFACTANTS AND DETERGENTS
·
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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LANGMUIR
·
2017
·
IF 3.833
Tingting Zhou,Jiagen Li,Xu Jia,Xubo Zhao,Peng Liu
Novel biocompatible and biodegradable pH/reduction dual-responsive oxidized alginate-doxorubicin (mPEG-OAL-DOX/Cys) prodrug nanohydrogels were designed for tumor-specific intracellular triggered release of anticancer drug DOX by conjugating DOX via acid-labile Schiff base linkage into the PEGylated oxidized alginate (mPEG-OAL) cross-linked with bioreducible disulfide bond. The effect of the complexation with cyclodextrins (α-CD and β-CD) before or after the cross-linking of the mPEG-OAL on the DOX content and controlled release performance was investigated. It was found that the cyclodextrin inclusion complex prodrug nanohydrogels mPEG(CD)-OAL-DOX/Cys, prepared by cross-linking of the mPEG-OAL after complexation with cyclodextrins, exhibited better pH/reduction dual-responsive controlled release performance than the mPEG-OAL-DOX/Cys(CD) ones prepared by cross-linking of the mPEG-OAL before complexation with cyclodextrins, owing to the supramolecular cross-linking of the adjacent pseudopolyrotaxanes. Especially for the cyclodextrin inclusion complex prodrug nanohydrogels mPEG(α-CD)-OAL-DOX/Cys, DOX was released rapidly under lower pH media mimicking the tumor microenvironment and completely released within 48 h, while the premature leakage under the simulated physiological condition was ∼40%, without burst release in both cases. The cellular toxicity and uptake results demonstrated that the mPEG(α-CD)-OAL-DOX/Cys prodrug nanohydrogels possessed similar inhibition against cancer cell growth in comparison with the free DOX and enhanced drug intracellular accumulation.
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RSC Advances
·
2017
·Vol. 7
·期 89
·56519-56527
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IF 3.108
Aihua Yao,Qingge Fu,Ling Xu,Yan Xu,Wenqi Jiang,Deping Wang
Poly(4-vinylpyridine) (P4VP), a pH-sensitive polymer, was employed to non-covalently functionalize graphene oxides (GOs) through π–π stacking interactions. Citrate-capped Au nanoparticles (Au NPs) were then immobilized onto the P4VP-grafted GO, yielding pH-responsive Au NPs–GO nanocomposites. Such Au NPs–GO nanocomposites displayed pH-responsive localized surface plasmon resonance (LSPR) changes and assembly behavior due to protonation and deprotonation of the pyridine units of P4VP molecules. The catalytic activity of the Au NPs–GO nanocomposites was evaluated using the reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) as a model reaction, and demonstrated significantly high catalytic activity and stability at low pH (2.0), which was 4-fold higher than that at high pH (5.0). Furthermore, our results indicated that the Au NPs–GO nanocomposites induced active adsorption and selective SERS detection of negatively charged analytes under low pH conditions, and are therefore highly attractive for real-world chemical detection.
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ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Hongmei Li,Xing Qian,Chong Xu,Shaowei Huang,Changli Zhu,Xiancai Jiang,Li Shao,Linxi Hou
The development of highly active and stable earth-abundant electrocatalysts to reduce or eliminate the reliance on noble-metal based ones for hydrogen evolution reaction (HER) over a broad pH range remains a great challenge. Herein, hierarchical porous Co9S8/N-doped carbon@MoS2 (Co9S8/NC@MoS2) polyhedrons have been synthesized by a facile hydrothermal approach using highly conductive Co/NC polyhedrons composed of cobalt nanoparticles embedded in N-doped carbon matrices as both the structural support and cobalt source. The Co/NC polyhedrons were prepared by direct carbonization of Co-based zeolitic imidazolate framework (ZIF-67) in Ar atmosphere. Benefiting from the prominent synergistic effect of N-doped carbon enhancing the conductivity of the hybrid, MoS2 and Co9S8 providing abundant catalytically active sites as well as the well-defined polyhedral structure promoting mechanical stability, the as-synthesized Co9S8/NC@MoS2 shows excellent HER activity and good stability over a broad pH range, with onset overpotentials of 4, 38, and 45 mV, Tafel slopes of 60.3, 68.8, and 126.1 mV dec–1, and overpotentials of 67, 117, and 261 mV at 10 mA cm–2 in 1.0 M KOH, 0.5 M H2SO4, and 1.0 M phosphate buffer solution (PBS), respectively. This work provides a general and promising approach for the design and synthesis of inexpensive and efficient pH-universal HER electrocatalysts.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2017
·
IF 4.9
Hao Li,Yanbei Cao,Di Zhang,Bo Pan
The dominant adsorption mechanism of ionizable organic chemicals (IOCs) on carbonaceous materials is still unclear. This study used benzoic acid (BA), o -chlorobenzoic acid (2-CBA) and p -chlorobenzoic acid (4-CBA) as representatives of IOCs to investigate the dominant adsorption mechanism on graphene oxide (GO) and graphite (GP), with a specific emphasis on the impact of pH-dependent K OW . The order of apparent adsorption of the investigated chemicals changed with pH, which could not be explained by their constant K OW . According to our measurement, K OW varied greatly with pH. The pH-dependent adsorption of BA, 2-CBA and 4-CBA were significantly correlated with pH-dependent K OW for both GO and GP. Our observations indicated that the hydrophobic effects may dominate the apparent adsorption of BA, 2-CBA and 4-CBA on GO and GP. Electrostatic repulsion played a minor role in their reduced adsorption at high pH. Negative charge-assisted H-bond and π-π interactions may explain the adsorption of negatively charged BA, 2-CBA and 4-CBA on negatively charged GO. This study implied that pH-dependent K OW rather than constant K OW should be incorporated to understand IOC adsorption as affected by pH.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2017
·Vol. 44
·期 1
·491-502
·
IF 1.369
Li Shaoxin,Zhao Bing,Kan Wei,Wang Liyan,Song Bo,Chen Shuwen
A novel pH fluorescence probe (PIF), derived from phenanthro[9,10- d ]imidazole bound to the fluorescein, is designed and synthesized based on the intramolecular hydrogen bond and then its spectra properties are investigated. Probe PIF exhibits negligible fluorescence intensity at acidic pH condition due to ESIPT quenching caused by the formation of the intramolecular hydrogen bonds, and a significant fluorescence enhancement in neutral and weak alkaline environments because of the strengthened ICT process arose from the fracture of the intramolecular hydrogen bonds. The studies of UV–Vis and fluorescence spectra mean that probe PIF is able to respond linearly and reversibly over pH from 6.5 to 9.0 with p K
a of 7.0. Moreover, the pH responses of probe PIF are stable and not disturbed by the common cations and anions. The possible response mechanism has been proposed according to the analysis of 1 H NMR and DFT calculations.
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Polymer Chemistry
·
2017
·Vol. 8
·期 45
·7025-7032
·
IF 5.375
Jiang Xiao,Junyan Tan,Rujian Jiang,Xiongliang He,Yanzhi Xu,Ying Ling,Shifang Luan,Haoyu Tang
A homopolypeptide, namely poly(S-(2-carboxylethyl)-L-cysteine) (PCELC), with pH and redox dual responsiveness was prepared by ring-opening polymerization of S-(2-(methoxycarbonyl)ethyl)-L-cysteine based N-carboxyanhydride (MCELC-NCA) and subsequent hydrolysis. The pH-induced solution phase transition of PCELC was at pH = ∼4.50 as revealed by DLS and UV-vis spectroscopy. The thioether linkages of PCELC can be readily oxidized by H2O2 at 40 °C yielding PCELCox with sulfoxide and sulfone linkages as revealed by 1H NMR and FTIR. PCELCox also showed pH responsiveness with the variation of polymer aggregation sizes, but without solution phase separation. PCELCox can be partially reduced by 3-mercaptopropionic acid as suggested by 1H NMR and FTIR analysis. The pH-induced solution phase transition behavior of the reduction product (i.e., PCELCre) was different from that of the as-prepared PCELC. Moreover, PCELC can be used as a pH and oxidation dual responsive stabilizer to control the aggregation of single-walled carbon nanotubes (SWCNTs) in aqueous solution.
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POLYMER DEGRADATION AND STABILITY
·
2017
·
IF 3.386
Yue Wang,Ning Yang,Dandan Wang,Yang He,Li Chen,Yiping Zhao
The lack of identified binding sites for drugs and the undegradability limited the development of the thermo-sensitive hydrogels based on N-isopropylacrylamide (NIPAAm) in the intelligent drug delivery system (DDS). Therefore, the poly (Maleic anhydride-β-cyclodextrin- co -NIPAAm) (poly (MAH-β-CD- co -NIPAAm)) hydrogels were obtained to overcome these disadvantages. β-cyclodextrin (β-CD) with the drug inclusion properties and degradation capacity was modified by maleic anhydride (MAH) and the resultant monomer was fixed in the gel network by a series of polymerization reactions . The physical and chemical properties of the monomer and the poly (MAH-β-CD- co -NIPAAm) hydrogels were systemically investigated. The swelling/deswelling kinetics at different temperature and pH indicated that the gels exhibit dual responsiveness. The model drug naproxen sodium was identified by MAH-β-CD, so it was efficiently loaded on the hydrogels. The drug released in a controlled manner from the copolymerization hydrogels, especially displayed slower release efficiency in simulates stomach conditions. And these hydrogels also showed biodegradability in the presence of α-amylase. The above facts demonstrated that the poly (MAH-β-CD- co -NIPAAm) hydrogels was an effective oral drug system.
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