Acta Biomaterialia
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2018
·
IF 6.383
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.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2018
·Vol. 136
·期 10
·47160
·
IF 1.901
G. Lin,X. Chen,H. Zhou,X. Zhou,H. Xu,H. Chen
Feather keratin (FK) and carboxymethyl cellulose (CMC) were used as raw materials to prepare a FK/CMC polyelectrolyte complex via electrostatic interactions. Using avermectin (AVM) as a model drug and elevated temperature, an FK/CMC@AVM drug-carrying complex was obtained. The structure and morphology of FK/CMC@AVM were both analyzed by Fourier transform infrared spectroscopy, dynamic light scattering, and scanning electron microscopy (SEM). Furthermore, the encapsulation efficiency, anti-ultraviolet, sustained release, and toxicity properties of FK/CMC@AVM were studied. The results showed that the average particle size of FK/CMC@AVM was 386.57 nm and the encapsulation efficiency was 67.06%. Under UV light irradiation, FK/CMC@AVM significantly improved the stability of AVM and the half-life of AVM was found to be delayed from 354 to 1800 min. Moreover, the sustained release of AVM featured pH sensitivity and was consistent with the Korsmeyer–Peppas model. Upon increasing the pH from 1.5 to 9.5, the release mechanism of AVM changed from Fick diffusion to non-Fick diffusion. Finally, the toxicity characteristics of FK/CMC@AVM were not significantly different from those of nonmodified AVM. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47160.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2018
·Vol. 135
·期 34
·46626
·
IF 1.901
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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CARBOHYDRATE POLYMERS
·
2018
·
IF 5.158
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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TALANTA
·
2018
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IF 4.244
Yang Shu,Rusheng Song,Anqi Zheng,Jingli Huang,Mingli Chen,Jianhua Wang
A thermo/pH dual-stimuli-responsive drug delivery system (DDS) based on polymer coated mesoporous silica nanostructures (MSNs) is developed for facilitating chemotherapy and photothermal therapy. Thermo/pH-responsive polymer, poly((N-isopropylacrylamide, NIPAM)- co -methacrylic acid, MA), is grafted onto MSNs by in situ polymerization, followed by loading a chemotherapeutic drug (doxorubicin hydrochloride, DOX) and a near-infrared-absorbing phototherapeutic agent (indocyanine green, ICG) to construct the intelligent drug delivery system, shortly as [email protected] (NIPAM- co -MA). At NIR irradiation, the photothermal conversion capability of ICG raises the temperature of the DDS and opens the gatekeeper by shrinkage of the copolymer p(NIPAM- co -MA), which triggers controlled release of DOX at an elevated temperature. On the other hand, drug release is also realized at pH 5.3, a characteristic pH value in cancer cell microenvironment, at which it not only causes the shrinkage of the pH-sensitive polymeric moiety of methacrylic acid in [email protected] (NIPAM- co -MA) but also deteriorates electrostatic interaction of DOX molecules in the mesoporous channel by protonation of silanols . In addition, ICG further ensures photothermal therapy (PTT) and photodynamic therapy (PDT). The cytotoxicity assay of HeLa cells shows obvious synergistic effect by demonstrating that the combined use of DOX and ICG is more effective in killing HeLa cells than free DOX and ICG. The endocytosis of the drug is monitored by cell imaging.
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RSC Advances
·
2018
·Vol. 8
·期 4
·2082-2091
·
IF 2.936
Yangui Chen,Xiaoxia Li,Hong Xiao,Jinpeng Xiao,Bo Li,Xiaoyan Chen,Yong Wang,Du Cheng,Xintao Shuai
Owing to the complexity of tumorgenesis, combination therapy has proven to be a viable strategy for cancer treatment in recent years. However, the delivery and site-specific release of different therapeutic agents remain a major challenge in combination therapy. In this study, a polymeric nanovesicle based on a copolymer of polyethylene glycol and a polypeptide derivative was introduced as a vector to simultaneously deliver hydrophobic gefitinib and hydrophilic doxorubicin hydrochloride for multi-target combination therapy. The vesicle incorporating the two drugs exhibited prominent pH/reduction sensitivities to trigger the release of gefitinib and doxorubicin inside cancer cells. The two drugs co-delivered by the polymeric nanovesicle exhibited a joint anticancer effect both in vitro and in vivo. In particular, a remarkable therapeutic effect was demonstrated in animal studies using a mouse N2a neuroblastoma model. This study reveals the potential of reduction and pH dual-responsive nanovesicles bearing gefitinib and doxorubicin as an effective nano-medicine for cancer treatment.
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高影响因子
Catalysts
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2018
·Vol. 8
·期 1
·13
·
IF 3.465
Li Xu,Guli Cui,Caixia Ke,Yanli Fan,Yunjun Yan
A kind of pH-responsive particle was synthesized using modified pullulan polysaccharide. The synthesized particle possessed a series of merits, such as good dispersity, chemical stability and variability of particle size, making it a suitable carrier for enzyme immobilization. Then,Burkholderia cepacialipase (BCL), a promising biocatalyst in transesterification reaction, was immobilized on the synthesized particle. The highest catalytic activity and immobilization efficiency were achieved at pH 6.5 because the particle size was obviously enlarged and correspondingly the adsorption surface for BCL was significantly increased. The immobilization enzyme loading was further optimized, and the derivative lipase was applied in chiral resolution. Under the optimal reaction conditions, the immobilized BCL showed a very good performance and significantly shortened the reaction equilibrium time from 30 h of the free lipase to 2 h with a conversion rate of 50.0% andeesat 99.2%. The immobilized lipase also exhibited good operational stability; after being used for 10 cycles, it still retained over 80% of its original activity. Moreover, it could keep more than 80% activity after storage for 20 days at room temperature in a dry environment. In addition, to learn the potential mechanism, the morphology of the particles and the immobilized lipase were both characterized with a scanning electron microscope and confocal laser scanning microscopy. It was found that the enlarged spherical surface of the particle in low pH values probably led to high immobilized efficiency, resulting in the improvement of enantioselectivity activity in chiral resolution.Keywords:immobilization;Burkholderia cepacialipase;chiral resolution;1-phenylethanol;pullulan
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CELLULOSE
·
2018
·Vol. 25
·期 10
·5687-5696
·
IF 3.809
Liu Shaojie,Sun Tingting,Yang Desheng,Cao Meng,Liang Huazhe
Abstract Water-soluble polyacrylic acid was prepared by solution polymerization, and then partially acylated by SOCl 2 to give a random copolymer of poly(acrylic acid- co -acryloyl chloride) (P(AA- co -AC)). Through the reaction of acyl chloride groups in P(AA- co -AC) with hydroxyl groups in 4-hydroxy-2,2,6,6-tetramethyl-piperidinooxy (4-OH-TEMPO), the water-soluble TEMPO immobilized copolymer of poly(acrylic acid- co -2,2,6,6-tetramethylpiperidinyloxy-4-yl-acrylate) (P(AA- co -TA)) with different TEMPO loadings were prepared and characterized by Fourier transform infrared spectroscopy and conductometric titration. P(AA- co -TA) was used as a recoverable catalyst instead of free TEMPO for selective catalytic oxidation of cellulose in water. The carboxyl content of oxidized cellulose with P(AA- co -TA) as catalyst was up to 60% of the free TEMPO level. Furthermore, P(AA- co -TA) was easy to recycle by its pH-sensitivity and the activity did not decrease after 4 cycles. Graphical abstract
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ACS Applied Materials & Interfaces
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2018
·
IF 8.097
Yuqian Liu,Qingsheng Guo,Xiaojun Qu,Qingjiang Sun
The combination of functional nucleic acids and nanomaterials enables the continuous development of hybrid nanosystems that have found wide applications including chemo/biosensing. Herein, we report the supramolecular assembly of a “sesame biscuit”-like superstructural nanosystem based on aptamer, quantum dot (QD), and graphene oxide (GO), and its diverse applications in Pb2+ and pH sensing. The nanosystem was assembled via adsorbing silica-encapsulated green-emitting QD onto the edge of GO by ionic interaction, followed by absorbing aptamer-modified red-emitting QD onto the GO surface via the π-stacking interaction. The nanosystem showed the characteristic of the nonquenched green fluorescence due to silica encapsulation and quenched red fluorescence owing to nanomaterial surface energy transfer. The nanosystem responded to Pb2+/pH in ratiometric fluorescence: the red fluorescence varied upon analyte-driven conformational changes of the aptamer, whereas the green one remained constant. Under optimized conditions, the nanosystem was demonstrated to be capable of quantifying Pb2+ with a detection limit of 11.7 pM, as well as pH with a sensing resolution of 0.1 pH unit. More importantly, the ratiometric nanosystem facilitated visualization of analytes in a distinct “traffic light” manner, which was exemplified by semiquantification of exogenous Pb2+ in living cells. To demonstrate practicality, fluorescent test strips were fabricated by immobilizing the nanosystem on paper. The fluorescent test strips displayed traffic light-type fluorescence color changes, with the capacity for on-site, naked-eye detection of Pb2+ in real samples, as well as point-of-care pH testing in routine urinalysis.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2018
·Vol. 20
·期 30
·19900-19905
·
IF 3.906
Caili Dai,Qianru Yang,Mingwei Gao,Mingwei Zhao,Jianfeng Jiang
To indicate the difference between pH and CO2 stimuli mechanisms, a dual responsive system is constructed with the aid of N-[3-(dimethylamino)propyl]docosanamide (NDPD) and sodium salicylate (NaSal), which is responsive to pH and CO2. The dual responsive system is characterized by rheometry, cryo-TEM and 1H NMR spectroscopy. After bubbling CO2 or adjusting the pH, the rheological properties indicate the formation of wormlike micelles. The cyro-TEM images also confirmed wormlike micelles. The effect of temperature is also clarified. By comparing the rheological properties of the wormlike micelles with pH and CO2 stimuli conditions, combined with cryo-TEM and 1H NMR results, the stimuli mechanisms of pH and CO2 to the dual responsive system are shown. Through this work, we expect to deepen our understanding of the responsiveness of a self-assembled system.
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ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Kaijun Li,Ruiquan Yu,Ruixin Zhu,Ruifeng Liang,Gongyan Liu,Biyu Peng
In this work, pH-sensitive and chromium-loaded mineralized nanoparticles (Cr-PPA NPs) were developed by self-assembly of poly (poly(ethylene glycol) methyl ether acrylate-co-acrylic acid) (poly(PEG-co-AA)) copolymers templated Cr(OH)3 mineralization. The Cr-PPA NPs exhibit excellent colloidal stability in water with high salt concentration, protein, and pH above 3.0. As a novel chrome tanning agent, such Cr-PPA NPs could effectively protect and deliver chromium into pickled pelt without reacting with collagen fibers during the penetration process, due to its antifouling PEG surface and nanosize. When the interior pH of the pickled pelt was lower than 2.5, the dissolution of the mineralized Cr(OH)3 core would cause disassembly of Cr-PPA NPs and rapid release of Cr3+ ions, leading to uniform chromium distribution in leather. After basifying, the released Cr3+ ions would cross-link the carboxyl groups both on collagen fibers and poly(PEG-co-AA) copolymers, resulting in chromium adsorption efficiency in leather higher than 90% and less chromium discharge in wastewater. Simultaneously, the resultant leather was given enhanced hydrothermal stability and physical properties based on above efficient chromium cross-linking. Compared with traditional chrome tanning agent, this pH-sensitive Cr-PPA NPs can really break through the existing balance limitation between chromium penetration and combination in the conventional tanning process and become a promising strategy for cleaner leather production.
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LANGMUIR
·
2018
·
IF 3.789
Baoqing Liu,Xuefei Lu,Ze Qiao,Liping Song,Qian Cheng,Jiawei Zhang,Afang Zhang,Youju Huang,Tao Chen
Two-dimensional (2D) gold nanoparticle (Au NP) monolayer film possesses a lot of fascinating peculiarities, and has shown promising applications in photoelectrical devices, catalysis, spectroscopy, sensors, and anticounterfeiting. Because of the localized surface plasmon resonance (LSPR) property predetermined by the natural structure of metal nanoparticles, it is usually difficult to realize the reversible LSPR transition of 2D film. In this work, we report on the fabrication of a large-area free-standing Au NP monolayer film with dual-responsive switchable plasmonic property using a pH- or thermal-responsive dendronized copolymer as a stimuli-sensitive linker. In this system, an oligoethylene-glycol-based (OEG-based) dendronized copolymer (named PG1A) with pH or temperature sensitivity was first modified onto the surface of a Au NP. Then, polyethylene glycol dibenzyl aldehyde (PEG-DA) was introduced to interact with the amino moieties from PG1A before the process of oil–water interfacial self-assembly of NPs, resulting in an elastic, robust, pH- or temperature-sensitive interpenetrating network among Au NPs in monolayer films. In addition, the film could exhibit reversibly plasmonic shifts of about 77 nm and inherent color changes through varying temperature or pH. The obtained free-standing monolayer film also shows an excellent transferable property, which can be easily transferred onto substrates such as plastic molds, PDMS, copper grids, and silicon wafers. In virtue of these peculiarities of the free-standing property, special plasmonic signal, and homologous macroscopic color, the transferred film was primely applied to an anticounterfeiting security label with clear color change at the designed spots, providing a new avenue to plasmonic nanodevices with various applications.
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高影响因子
危险品化学品经营许可证（带存储）