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CARBOHYDRATE POLYMERS · 2021 · IF 9.381

O-carboxymethyl chitosan based pH/hypoxia-responsive micelles relieve hypoxia and induce ROS in tumor microenvironment

Liqun Jiang,Mi Zhang,Yuting Bai,Feiyan Cui,Cong Zhang,Ziyao Wang,Sujia Si,Ling Yang,Yun Wang,Yudong Zhang,Lei Li,Shuo Liu,Xiangrong Wei,Yan Wang,Ya Xu,Jian Meng

The hypoxia in tumor microenvironment (TME) can upregulate the HIF-1α and PD-L1 expression and cause immunosuppression of tumor. In this study, a carboxymethyl chitosan-based pH/hypoxia-responsive and γ-Fe 2 O 3 /isosorbide dinitrate carrying micelle was designed, and it could catalyze endogenous H 2 O 2 to generate oxygen and relieve hypoxia in TME, so as to relieve the overexpression of HIF-1α and PD-L1 in tumor; meanwhile, it could react with H 2 O 2 to release ROS via Fenton reaction and induce cytotoxicity in tumor. Along with these multiple effects, this carboxymethyl chitosan-based micelles could provide a comprehensive strategy for tumor treatment.

CAS / MDL: 1309-37-1
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY · 2021 · IF 3.981

ZnO QD covalently coated, GSH/pH dual-responsive drug delivery system for chemotherapeutic/ionic synergistic therapy

Bo Fu,Can Tao,Nian Chen,Jie-Rou Lin,Ping Zhao

Chemotherapeutical agents have been frequently reported to have adverse side effects which reduce their application in clinic. Herein, we reported a mesoporous silica nanoparticles (MSNs)-based drug delivery system (DDS) capped with zinc oxide quantum dots (ZnO QD) which has glutathione (GSH)/pH dual-responsive controlled release in the cancer cells. The drug loaded DDS have higher cellular inhibition than the free drug because of the synergistic effect of payload DNM and the Zn 2+ dissolved from ZnO QD. The anti-cancer mechanism research indicates that the designed drug loaded DDS can cause mitochondrial damage, arrest the cell cycle and induce the cell apoptosis and autophagy. The combination of excellent biocompatibility , selective release performance, synergistic cellular cytotoxicity, endowed the DDS with the potential of utilization in cancer treatment.

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SENSORS AND ACTUATORS B-CHEMICAL · 2019 · IF 6.393

Quercetin@ZIF-90 as a novel antioxidant for label-free colorimetric ATP sensing at neutral pH

Xin Xu,Danyang Nan,Huan Yang,Shuang Pan,Hui Liu,Xiaoli Hu

Quercetin is a nature polyphenolic flavonoid compound, which act as antioxidant and radical scavengers in cells. However, such activities strongly depend on the intracellular microenvironment, which has become an urgency to develop a more stable method for better use of quercetin. Herein, we report a facile approach to fabricate Quercetin@ZIF-90 (QZ) with a narrow size distribution about 100 nm, the synthesized QZ exhibits considerable antioxidant and radical scavenger ability comparing to bare quercetin. Moreover, the experiment results indicated that QZ was sensitive to adenosine 5′-triphosphate (ATP) and pH, thus QZ was applied as a novel antioxidant for the determination of ATP. In brief, though 3, 3′, 5, 5′-tetramethylbenzidine (TMB) could be oxidized to blue cation radical complex by oxidase-like BSA-MnO 2 nanosheets (MNs) at neutral pH, QZ could sufficiently protect against MNs-induced TMB cation radicals reaction, which means no obvious color change in MNs-TMB system after the addition of QZ. However, ATP could induced collapse of QZ due to the interaction between ATP and Zn 2+ allowing the release of quercetin from ZIF-90 shell, and the inhibition effect to the MNs was weakened, leading to the recovery of blue oxTMB. In this way, a novel “Off-On” colorimetric method for ATP sensing was established, and the method displayed a good linear relationship ranging from 2.0 μ mol L −1 to 80.0 μ mol L −1 . The reported strategy is also capable of ATP sensing in MCF-7 cell lysates, which illustrated our method exhibited high sensitivity and selectivity.

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ADVANCES IN POLYMER TECHNOLOGY · 2020 · IF 1.539

Synthesis of Polymer Assembled Mesoporous CaCO3 Nanoparticles for Molecular Targeting and pH-Responsive Controlled Drug Release

Jinjing Xing,Yeqiang Cai,Yikun Wang,Haifu Zheng,Yujia Liu

CaCO3 nanoparticles are very suitable as intelligent carriers because of their ideal biocompatibility and biodegradability, especially their sensitivity to pH. In this paper, we use mesoporous CaCO3 nanoparticles as intelligent carrier, sodium alginate, and chitosan as alternating assembly materials, folic acid as target molecules, and exploit layer-by-layer assembly technology to achieve sensitive molecular targeting and pH response drug release. Mesoporous CaCO3 hybrid nanoparticles have high drug loading on doxorubicin. The effects of different pH values on drug release in vitro were studied by regulating simulated body fluids with different pH values. The cytotoxicity, targeting effect, and drug release of human cervical cancer cell line (HeLa) were studied by cell vitality and imaging experiments. All the evidence suggests that the smart mesoporous CaCO3 nanoparticles may be a potential clinical application platform for cancer therapy.

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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2020 ·Vol. 167 ·期 2 ·027508 · IF 3.721

An ON/OFF Aptasensor for Detection of AFB1 Based on pH-sensitive Polymer and GO Composite

Kaili Cui,Guanghan Li,Luyan Wang,Wenjuan Guo,Meishan Pei

In this work, a novel ON/OFF aptasensor was designed with a composite film consisting of carboxylated graphene oxide (GO) and poly(4-vinyl pyridine) (P4VP) for the accurate and sensitive detection of AFB1. The "on" and "off" behavior of the electrochemical sensor could be controlled by the pH sensitive P4VP. Through continuous switching of solution pH value below and above pKa of P4VP (pKa = 4.9), the conversion in the reversible electron transfer between protonized or deprotonized P4VP and the electrochemical probe was used to control the "ON" and "OFF" state of the electrochemical sensor. The condition was optimized when the electrochemical sensor is kept "ON" state, finding that the aptasensor showed highest current signal and the best electrochemical performance at pH = 4. Here the addition of P4VP not only could significantly improve the current signal at pH = 4 but also increase the stability of the modified electrode. Carboxylated GO was able to form an amide linkage with an amino-modified aptamer to fix the aptamer more firmly and increase the immobilized quantity of aptamer. On the basis of the excellent electrochemical performance of GO-P4VP composite, the designed biosensor exhibited a wide linear range from 0.01 to 50 ng ml−1 and a low detection limit of 14.75 pg ml−1.

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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

Preparation of macroporous polyvinyl alcohol formaldehyde based hydrogels and their dual thermo- and pH-responsive behavior

Kai Shi,Zhi Liu,Yanxiong Pan,Baolong Wang,Jiuduo Xu,Di Sha,Xu Yang,Xiangling Ji

Dual thermo- and pH-responsive polymer hydrogels have broad potential applications due to their unique responsive behavior to environmental stimuli   regulated   by more than one mechanism. Herein, the dual thermo- and pH-responsive polyvinyl alcohol formaldehyde (PVF) based hydrogels were successfully prepared via redox grafting polymerization by incorporating respectively poly(N-isopropylacrylamide) (PNIPAM) and poly(acrylic acid) (PAA) moieties onto PVF backbone. These hydrogels retain an interconnected macroporous structure with high porosity (~83.0%), facilitating rapid penetration and diffusion of water molecules. The sizes of pore and pore walls are in micrometer scale, significantly reducing the characteristic time of swelling or deswelling. Besides, these hydrogels possess the thermo-responsiveness even in high grafting percentage of PAA (60.8%), overcoming the inhibition effect of PAA moieties in a high content on thermal sensitivity of traditional poly(NIPAM-co-AA) copolymers. Their pH-responsiveness and excellent repeated absorption performance are determined by measuring the absorption capacities of hydrogels in water and different buffer solutions. Moreover, these hydrogels exhibit rapid deswelling kinetics on the minute time scale by detecting water retention in pH 3 buffer solution at 50 °C. In addition, the deswelling behavior leads to the noticeable changes of macroscopic dimensions of hydrogels; we anticipate potential applications in dual thermal and pH sensors.

CAS / MDL: 16774-21-3 9002-93-1
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Advanced Materials Interfaces · 2019 ·Vol. 7 ·期 1 ·1901535 · IF 4.713

Self-Regulating Cross-Linked Graphene Oxide Membranes with Stable Retention Properties over a Wide pH Range

Guoke Zhao,Hongwei Zhu

To extend the effective working range of porous membranes is highly desirable for membrane applications. Here, graphene oxide (GO) based membranes capable of retaining stable retention properties with varying pH are reported. The self-adjustable properties of GO based membranes are realized by coupling with pH-responsive polyacrylic acid (PAA) molecules via a facile vacuum filtration process. With decreasing pH, the shrinkage of the molecular chains of PAA decreases the interlayer spacing of PAA/GO membranes, which compensates for the weakened Donnan effect in acidic conditions, leading to the stable retention properties of the membranes over a wide pH range. With PAA introduced, the laminated structure of the membranes is well preserved while the membrane thickness is slightly increased. PAA endows the membranes with obvious self-alteration of pore structure in response to the change of pH. Nanofiltration performance measurements show that the dye retention properties of GO membranes decrease sharply when the pH changes from 9 to 1. However, the rejection rates of PAA/GO membranes could be well retained or even increased in acidic conditions. This work demonstrates that PAA is an effective pH-sensitive modification material for fabricating GO-based membranes with stable retention properties under varying pH.

CAS / MDL: 7429-91-6 7439-98-7
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JOURNAL OF DAIRY SCIENCE · 2019 · IF 3.082

Change in the structural and functional properties of goat milk protein due to pH and heat

X.Y. Li,M. Cheng,J. Li,X. Zhao,Y.S. Qin,D. Chen,J.M. Wang,C.F. Wang

ABSTRACT This study was carried out to investigate the effects of pH and heat on the structure and function of milk proteins by comparing goat milk treated under different pH and temperature conditions. The results showed that pH had a significant effect on the thermal stability of goat milk proteins, and the proteins were least thermally stable at pH 7.7. Except for the pH 6.9 goat milk, the surface hydrophobicities of the milk proteins at various pH values reached their maxima at 85°C. The particle size, zeta potential, and content of regular secondary structure also decreased significantly at 85°C, and the turbidity of milk proteins under alkaline pH conditions was lower than that under acidic conditions. It was concluded that alkaline conditions resulted in better emulsion stability and oil-holding capacity, and acidic conditions offered better foaming ability, foam stability, and water-holding capacity for goat milk protein during heat processing. It can also be seen that 85°C was the key temperature for milk proteins after changing the pH of the milk. This paper provides a theoretical basis for optimizing the processing conditions for goat milk and the applications of goat milk proteins.

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ACS Applied Materials & Interfaces · 2019 · IF 8.456

An Environment-Friendly Fertilizer Prepared by Layer-by-Layer Self-Assembly for pH-Responsive Nutrient Release

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.

CAS / MDL: 8061-51-6
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CARBOHYDRATE POLYMERS · 2019 · IF 6.044

A novel pH-sensitive targeting polysaccharide-gold nanorod conjugate for combined photothermal-chemotherapy of breast cancer

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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Nanoscale · 2019 ·Vol. 11 ·期 19 ·9457-9467 · IF 6.97

pH/redox dual-stimuli-responsive cross-linked polyphosphazene nanoparticles for multimodal imaging-guided chemo-photodynamic therapy

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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CHEMISTRY-A EUROPEAN JOURNAL · 2019 ·Vol. 25 ·期 35 ·8353-8362 · IF 5.16

A pH-Sensitive Zwitterionic Iron Complex Probe with High Biocompatibility for Tumor-Specific Magnetic Resonance Imaging

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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