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JOURNAL OF ALLOYS AND COMPOUNDS · 2019 · IF 4.175

Reinforcing effects of waterproof substrate on the photo-, thermal and pH stabilities of perovskite nanocrystals

Xingyu Liu,Jinwei Gao,Wanqiang Liu,Qianming Wang

Lead halide perovskites have generated remarkable progress in a wide variety of opto-electronic fields. However, challenging issues including water-sensitive feature, poor stability over temperature change and mechanical fragility should be circumvented to enable the practical uses of such nanocrystals . Ethylene-propylene-diene monomer (EPDM) rubber, which possesses saturated and nonpolar polymeric chain, has been extensively explored in industry due to its sealing property, low-cost, dynamic and outstanding abrasive resistance. In this study, the hybrid inorganic-organic network with covalent cross-linkages and CsPbX 3 (X = Cl and Br) quantum dots has been established in EPDM rubber system via an effective and mild approach in the process of mixing reaction at room temperature. In contrast to pure perovskite dots, the peak emission intensity of CsPb(Cl 0·25 Br 0.75 ) 3 -EPDM can be well maintained after it has been immersed into aqueous solution for 2 h. Moreover, the water-mediated treatment will control the emission color evolution from cyan (485 nm) to green (510 nm) and such process can be fully reversible during the soaking and drying cycles. In addition, the employment of such polymeric host with superior heat resistance results in significant increases in thermal stability, mechanical strength and toughness. This efficient strategy will provide a rational design of reinforcing photoluminescence for all-inorganic perovskite quantum dots in numerous applications.

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LANGMUIR · 2019 · IF 3.683

Temperature and pH Responsive Janus Silica Nanoplates Prepared by the Sol–Gel Process and Postmodification

Hong Chen,Wenxin Fu,Zhibo Li

During the process of emulsifying and hydrolyzing, reactive poly(3-(triethoxysilyl)propyl methacrylate)-b-polystyrene (PTEPM-b-PS) diblock copolymers can self-assemble and become cross-linked to form hollow spheres in situ with polystyrene on their inner surfaces. The addition of tetraethoxysilane (TEOS), which was hydrolyzed and condensed together with PTEPM block, can make those spheres as soft foldable capsules or hard hollow spheres depending on the amount of added TESO. Then postmodification, the surface-initiated Atom Transfer Radical Polymerization (ATRP) was applied to afford stimuli-responsive spheres, and the corresponding responsive Janus nanoplates (RJPs) were finally obtained by crushing those responsive hollow spheres (HSs) showing smart tunable emulsifiability and great potential in oily water purification. This facile method to fabricate HSs and RJPs could be used for preparing different Janus polymer-inorganic capsules and nanoplates with varied functions by changing the chemical composition of copolymer surfactants as well as the postmodification process.

CAS / MDL: 2210-25-5
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2019 · IF 3.131

Pickering emulsions synergistic-stabilized by amphoteric lignin and SiO2 nanoparticles: Stability and pH-responsive mechanism

Shuo Lu,Dongjie Yang,Miao Wang,Mengzhen Yan,Yong Qian,Dafeng Zheng,Xueqing Qiu

The pH-responsive O/W Pickering emulsions were stabilized by amphoteric lignin (AML) absorbed with SiO 2 nanoparticles via electrostatic interaction. AML was gained by quaternary ammonium modification of alkali lignin, and its structure was characterized by 1 H NMR. Fourier transform infrared spectroscopies and Zeta potential measurements were performed to investigate the interaction between AML and SiO 2 . The formed AML@SiO 2 compounds were utilized to prepare Pickering emulsions. The influences of AML concentration and pH on emulsions were studied by rheological measurements and Turbiscan Lab Expert stability index system. The pH-responsive mechanism of Pickering emulsions was investigated by Zeta potential, quartz crystal microbalance with dissipation, atomic force microscopy and three-phase contact angle. The results indicated that at the pH range of 3-4, AML was absorbed on SiO 2 to realize the in-situ hydrophobization of SiO 2 , forming stable Pickering emulsions. When pH was above 4, only a little amount of AML was absorbed on SiO 2 due to the strong electrostatic repulsion between them, resulting in unstable emulsions. The emulsions could be cycled at least 5 times between emulsification and demulsification as well as exhibited excellent salt tolerance.

CAS / MDL: 7631-86-9
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BIOSENSORS & BIOELECTRONICS · 2019 · IF 9.518

A close-packed imprinted colloidal array for naked-eye detection of glycoproteins under physiological pH

Wei Chen,Min Fu,Xixi Zhu,Qingyun Liu

According to the combination of colloidal crystals and molecular imprinting techniques, a novel close-packed imprinted colloidal array (CPICA) for naked-eye horseradish peroxidase (HRP) detection at physiological pH was proposed. The CPICA was fabricated by self-assemble of monodispersed HRP imprinted particles. The HRP imprinted particles were prepared based on surface imprinting technique and immobilized template strategy using 2,4-difluoro-3-formylphenylboronic acid (DFFPBA) as functional monomer which allowed the material binding of HRP at physiological pH (denoted as SiO 2 @DFFPBA/MIPs). The adsorption capacity of the SiO 2 @DFFPBA/MIPs for HRP was 1.16 μmol/g, and reached saturated adsorption within 25 min. The limit of detection (LOD) of the CPICA was 3.0 × 10 −13  mol/mL. In addition, the adsorption of HRP on the CPICA could be directly transferred into visible color changes and readable optical signals through the reflection peak shifts. The structure color of the CPICA changed from brilliant blue to dark red with an maximum red shift of 87 nm when the HRP concentration increased from 2.5 to 20.0 μmol/L. Moreover, the CPICA could be used to detect HRP from human serum sample, which demonstrated the promising application prospects in colorimetric sensors.

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POLYMER JOURNAL · 2019 ·Vol. 51 ·期 11 ·1211-1222 · IF 2.639

Hydrazone-linked soybean protein isolate-carboxymethyl cellulose conjugates for pH-responsive controlled release of pesticides

Liu Guanghua,Lin Guanquan,Tan Mingyi,Zhou Hongjun,Chen Huayao,Xu Hua,Zhou Xinhua

To improve the utilization of pesticides and reduce the amount of pesticides used, sustained-release nanoparticles were prepared. Soybean protein isolate (SPI) and carboxymethyl cellulose (CMC) were modified to obtain hydrazine-modified SPI and aldehyde-modified CMC, respectively, and SPI-CMC was prepared by the condensation of hydrazine and aldehyde groups, forming a hydrazone bond. SPI-CMC was heated and loaded with avermectin (AVM) to obtain AVM/SPI-CMC. The encapsulation efficiency property, anti-ultraviolet property, sustained-release characteristics, pH responsiveness, and toxicological profiles were studied. The particles in the formulation were spherical-like, with sizes ranging between 150 and 250 nm. The encapsulation efficiency increased with the addition of SPI, which reached 44.49% when SPI was added in a mass ratio of m SPI-HYD : m CMC-ALD  = 2:1. The percentage of remaining AVM in AVM/SPI-CMC was 31.47% higher than that in the AVM solution after UV irradiation for 43 h. Moreover, the nanoparticles were responsive to pH. SPI-CMC had no significant effect on the insecticidal toxicity of AVM. Environmental friendly SPI-CMC could protect and release pesticides continuously, which could improve the efficiency of pesticides.

CAS / MDL: 9004-32-4 7790-28-5
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ACS Omega · 2018 · IF 0

Synergistic pH and Temperature-Driven Actuation of Poly(NIPAM-co-DMAPMA)/Clay Nanocomposite Hydrogel Bilayers

Guorong Gao,Liufang Wang,Yang Cong,Zhenwu Wang,Yang Zhou,Rong Wang,Jing Chen,Jun Fu

Hydrogel actuators that deform in response to external stimuli have promising applications in diverse fields. It is desirable to develop robust hydrogels with multiple and synergistic stimuli responsiveness. This work reports on robust poly(NIPAM-co-DMAPMA)/clay hydrogel bilayers that undergo reversible and repeatable curling/uncurling in response to pH and/or temperature changes. The bilayers are fabricated by sequential synthesis of thermoresponsive N-isopropylacrylamide (NIPAM) and N-[3-(dimethylamino)propyl] methacrylamide (DMAPMA) monomers, which produces robust interface bonding between the layers. Different NIPAM/DMAPMA ratios were used between two gel layers to manipulate the asymmetric responsiveness, thus leading to curling/uncurling of bilayers upon exposure to stimuli. The hydrogel bilayers are fabricated into soft manipulators to grasp and release target objects by pH and temperature changes, and as artificial muscle to lift and move a hanging weight by synergistic pH and temperature stimuli. This work provides a new type of asymmetric responsive hydrogel bilayer with potential applications in biomimetic actuators.

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JOURNAL OF APPLIED POLYMER SCIENCE · 2018 ·Vol. 135 ·期 34 ·46626 · IF 1.901

Highly efficient adsorbent for organic dyes based on a temperature- and pH-responsive multiblock polymer

Zhenglong Yang,Sai Chen,Kangyu Fu,Xinyan Liu,Feng Li,Yuchuan Du,Peiting Zhou,Zhihao Cheng

The self-assembly behavior of amphiphilic block copolymers in selective solutions has many applications in environmentally responsive polymer materials. In this article, we report on a new amphiphilic, temperature and pH dual-responsive poly[2-dimethylaminoethyl methacrylate- co -(methyl methacrylate)]- b -poly[poly(ethylene glycol) methacrylate] [P(DMAEMA- co -MMA)- b -PPEGMA], which was synthesized via reversible addition–fragmentation chain-transfer polymerization. The structure, self-assembly behaviors, and process of organic dye adsorption were characterized by 1 H-NMR, ultraviolet–visible absorbance spectroscopy, and DLS measurements. P(DMAEMA- co -MMA)- b -PPEGMA was proven to be an outstanding adsorbent with excellent reversibility. Methyl red was released from the micelles as the pH value of the solution was adjusted to 4, and it could also be encapsulated again when the pH value was adjusted to 7.4 because of the sensitive pH-responsive ability. It is promising that the triblock polymer had a positive effect on dye adsorption for environmental protection. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 46626.

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LANGMUIR · 2018 · IF 3.789

Real-Time Adsorption of Exo- and Endoglucanases on Cellulose: Effect of pH, Temperature, and Inhibitors

Peiqian Zhang,Mimi Chen,Yuhao Duan,Renliang Huang,Rongxin Su,Wei Qi,Wim Thielemans,Zhimin He

Effective regulation of cellulase adsorption is key to improving the efficiencies of the two major bottlenecks of lignocellulose hydrolysis and cellulase recovery. In this work, we investigated the effect of inhibitors, pH, and temperature on the adsorption of exo- and endoglucanases (Cel7A and Cel7B, respectively) on cellulose using quartz crystal microgravimetry with dissipation. The addition of glucose and cellobiose can both inhibit the hydrolysis activity of Cel7A, whereas only cellobiose can inhibit that of Cel7B. Notably, the adsorption was favored by acidic conditions (pH ≤ 4.8) and low temperature, whereas alkaline conditions (pH 9 and 10) facilitated enzyme desorption, which is useful to guide the process of cellulase recovery. The adsorption and hydrolysis activity of Cel7A and Cel7B were both higher at 45 °C than at 25 °C. These findings pave the way to effective regulation of cellulase adsorption and thus improve lignocellulose conversion and cellulase recovery.

CAS / MDL: 528-50-7 28072-80-2
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2018 · IF 5.091

pH-activatable polymeric nanodrugs enhanced tumor chemo/antiangiogenic combination therapy through improving targeting drug release

Hui Xiong,Yuanyuan Wu,Zhijie Jiang,Jianping Zhou,Min Yang,Jing Yao

It was widely accepted that polymeric nanodrugs held superiority in enhancing antitumor efficacy, reducing side effect and achieving better long-term prognosis. However, there still existed disputes that whether their therapeutic efficiency was closely related to insure effective release of hydrophobic drug located in their hydrophobic core in tumor site. In order to investigate this controversy, we constructed two polymeric nanodrugs (pH-activatable sLMWH-UOA and non-sensitive LMWH-UOA) with low molecular weight heparin (LMWH) and ursolic acid (UOA) for chemo-and anti-angiogenic combination therapy in hepatocellular carcinoma. The degradation ratio of pH-activatable sLMWH-UOA increased by 33% compared with non-sensitive LMWH-UOA in in vitro degradation study. Besides, confocal microscopy captured that sLMWH-UOA could effectively release drug in acidic microenvironment of lysosome while LMWH-UOA nearly could not. More importantly, in contrast with LMWH-UOA, sLMWH-UOA presented pH-dependent cytotoxicity, indicating that promoting drug release played a key role in enhancing the cytotoxicity of polymeric nanodrugs. Additionally, in vivo pharmacodynamic evaluation showed that although non-sensitive LMWH-UOA had benefited from enhanced tumor targeting drug delivery ability to achieve absolute advantage over free drug combination therapy in antitumor combination therapy, sLMWH-UOA could acquire further optimized combined therapeutic effect with better drug release in tumor. All above, application of tumor-triggered chemical bonds to construct polymeric nanodrugs held vast prospect for improving the therapeutic efficiency for tumor cells.

CAS / MDL: 123-08-0
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Acta Biomaterialia · 2018 · IF 6.383

PEGylated hydrazided gold nanorods for pH-triggered chemo/photodynamic/photothermal triple therapy of breast cancer

Weijun Xu,Junmin Qian,Guanghui Hou,Yaping Wang,Jinlei Wang,Tiantian Sun,Lijie Ji,Aili Suo,Yu Yao

Integration of multimodal therapies into one nanoplatform holds great promise to overcome the drawbacks of conventional single-modal therapy and pursues enhanced anticancer efficacy. Herein, we developed a PEGylated gold nanorods (GNRs)-based nanoplatform (GNRs-MPH -ALA/DOX -PEG) with pH-responsive drug release property for triple-combined chemotherapy (CT), photodynamic therapy (PDT) and photothermal therapy (PTT) of breast cancer. GNRs were first decorated with mercaptopropionylhydrazide (MPH) and thiol-terminated monomethoxyl poly(ethylene glycol) (mPEG-SH) via Au-thiol linkage, and subsequently conjugated with chemotherapeutant doxorubicin (DOX) and pro-photosensitizer 5-aminolevulinic acid (ALA) through acid-liable hydrazone bonds between drugs and MPH molecules. The resulting nanoplatform GNRs-MPH -ALA/DOX -PEG exhibited excellent stability in physiological solutions and pH-responsive DOX and ALA release behaviors. In vitro studies showed that GNRs-MPH -ALA/DOX -PEG could efficiently enter human breast cancer MCF-7 cells and release DOX and ALA into cytoplasm. Furthermore, DOX could locate in the cell nucleus and ALA was productively metabolized into protoporphyrin IX (PpIX). Upon near-infrared (NIR) irradiation, PpIX produced enough reactive oxygen species for PDT and meanwhile GNRs could efficiently induce hyperthermia for PTT. Compared with single CT and dual-modal CT/PDT or CT/PTT treatment, the triple-combined CT/PDT/PTT treatment could more efficiently kill MCF-7 cells via a superadditive antitumor effect. Furthermore, the circulation half-life of GNRs-MPH -ALA/DOX -PEG in the blood was as long as approximately 52 min and it exhibited a tumor accumulation of 3.3%. The triple-combined CT/PDT/PTT treatment could completely suppress tumor growth without obvious systemic toxicity. Our study paves a new avenue for multimodal therapy of breast cancer. Statement of significance The development of a simple but effective strategy to construct a versatile nanoplatform for multi-combined therapy still remains an enormous challenge. In this work, we developed a novel and simple nanoplatform GNRs-MPH -ALA/DOX -PEG with pH-responsive drug release for triple-combined chemotherapy (CT), photodynamic therapy (PDT) and photothermal therapy (PTT) of breast cancer. The nanoplatform could be efficiently internalized by MCF-7 cells. The intracellular GNRs-MPH -ALA/DOX -PEG could release DOX for CT, induce hyperthermia for PTT and generate high levels of ROS for PTT. Compared with single CT and dual-modal CT/PDT or CT/PTT treatments, the triple-combined CT/PDT/PTT treatment could more efficiently kill MCF-7 cells via a superadditive antitumor effect. Furthermore, upon triple-combined CT/PDT/PTT treatment, the tumor growth was completely suppressed without obvious systemic toxicity.

CAS / MDL: 1077-28-7
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Polymers · 2018 ·Vol. 10 ·期 11 ·1272 · IF 2.935

ZnO Quantum Dots Modified by pH-Activated Charge-Reversal Polymer for Tumor Targeted Drug Delivery

Yifan Wang,Liang He,Bing Yu,Yang Chen,Youqing Shen,Hailin Cong

In this paper, we reported a pH responsive nano drug delivery system (NDDS) based on ZnO quantum dots (QDs) for controlled release of drugs. Zwitterionic poly(carboxybetaine methacrylate) (PCBMA) and poly(2-(dimethylamino) ethyl methacrylate) (PDMAEMA) were introduced to modify ZnO QDs, which can help enhance water stability, increase blood circulation time, and promote endocytosis. After tuning of PCBMA/PDMAEMA ratios, the ZnO@P(CBMA-co-DMAEMA) nanoplatform shows a sensitive switch from strong protein adsorption resistance (with negatively charged surface) at physiological pH to strong adhesion to tumor cell membranes (with positively charged surface) at the slightly acidic extracellular pH of tumors. Anti-cancer drug, Doxorubicin (DOX), molecules were demonstrated to be successfully loaded to ZnO@P(CBMA-co-DMAEMA) with a relatively large drug loading content (24.6%). In addition, ZnO@P(CBMA-co-DMAEMA) loaded with DOX can achieve lysosomal acid degradation and release of DOX after endocytosis by tumor cells, resulting in synergistic treatment of cancer, which is attributed to a combination of the anticancer effect of Zn2+and DOX.Keywords:Zinc oxide quantum dots (ZnO QDs);poly(carboxybetaine methacry late) (PCBMA);poly(2-(dimethylamino) ethyl methacrylate) (PDMAEMA);drug delivery

CAS / MDL: 25316-40-9 79-41-4
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CARBOHYDRATE POLYMERS · 2018 · IF 5.158

One-pot construction of cellulose-gelatin supramolecular hydrogels with high strength and pH-responsive properties

Qilin Lu,Songhua Zhang,Mingcheng Xiong,Fengcai Lin,Lirong Tang,Biao Huang,Yandan Chen

Inspired by the supramolecular structure of cellulose, cellulose-gelatin supramolecular hydrogels with high strength and pH-sensitivity were constructed in a basic-based solvent system, ethylene diamine/potassium thiocyanate (EDA/KSCN) with the aid of cyclic freezing-thawing. The investigation on the characteristics of supramolecular hydrogels revealed that repeated freezing-thawing cycles played an important role in the formation of the physical cross-linked supramolecular network structure between cellulose and gelatin. The mechanical properties of supramolecular hydrogels were much higher than pure cellulose and gelatin hydrogel, and the compressive strength was 9.6 times higher than that of pure gelatin hydrogel. The synergistic effect between hydrogen-bonding interaction and the reinforcement of regenerated cellulose nanofibrils (CNF) contributed to the superior mechanical performance. Furthermore, the swelling kinetics tests showed that the supramolecular hydrogels exhibited excellent pH-responsibility, indicating potential applications in biomedical fields. Thus, a straightforward route to construct natural polymer-based hydrogels with supramolecular structure through physical crosslinking strategy without employing hazardous crosslinking agents was developed, paving the way for the design of new types of hydrogels.

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