SENSORS AND ACTUATORS B-CHEMICAL
·
2017
·
IF 5.401
Yu Cheng,Kai Ren,Dian Yang,Jie Wei
In this study, we propose a fluorescent bilayer hydrogel soft actuator that responds quickly to multiple environmental stimuli. The two layers of hydrogel contain poly(N-isopropylacrylamide) and poly(2-(dimethylamino) ethyl methacrylate), respectively, which enable their mechanical response to temperature and pH. Additionally, both hydrogel layers contain poly(ethylene oxide) diacrylate, which serves as the crosslinker. Thanks to the anisotropic swelling of two layers, the bilayer hydrogel structure exhibits rapid, reversible, and repeatable bending motion, under varying temperature or pH. In addition, a photo-sensitive coumarin-based unit is introduced into the hydrogel network to add fluorescence. A four-arm gripper made of hydrogel bilayers demonstrates rapid actuation in response to both temperature and pH. Furthermore, we design a circuit switch using the hydrogel bilayer to serve as one “bidirectional alarm” and selectively turn on light emitting diodes in different media. This work demonstrates the applications of the hydrogel bilayer as a soft actuator and a circuit switch in ionic circuitry, enabling potential applications in a wide range of fields, including biomimetic devices, biocompatible/medical devices, and environmental sensors.
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Advanced Healthcare Materials
·
2017
·Vol. 6
·期 19
·1700470
·
IF 5.11
Kai Han,Wei-Yun Zhang,Jin Zhang,Zhao-Yu Ma,He-You Han
Both excess dosages of drug and unwanted drug carrier can lead to severe side effects as well as the failure of tumor therapy. Here, an Fe 3+ –gallic acid based drug delivery system is designed for efficient monitoring of drug release in tumor. Fe 3+ and polyphenol gallic acid can form polygonal nanoscale coordination polymer in aqueous solution, which exhibits certain antitumor effect. Importantly, this coordination polymer possesses extremely high doxorubicin (DOX) loading efficacy (up to 48.3%). In vitro studies demonstrate that the fluorescence of DOX can be quenched efficiently when DOX is loaded on the coordination polymer. The acidity in lysosome also triggers the release of DOX and fluorescence recovery simultaneously, which realizes real-time monitoring of drug release in tumor cells. In vivo studies further indicate that this polyphenol-rich drug delivery system can significantly inhibit tumor growth with negligible heart toxicity of DOX. This system with minimal side effects should be a promising nanoplatform for tumor treatment.
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JOURNAL OF MATERIALS RESEARCH
·
2017
·Vol. 32
·期 4
·717-725
·
IF 1.673
D.D. Men,F. Zhou,H.L. Li,L.F. Hang,X.Y. Li,D.L. Liu,W.P. Cai,L.M. Qi,L.B. Li,Y. Li
A free standing 2D PS colloidal crystal with Au nanoshells/hydrogel composite film (CAuHCF) was fabricated by embedding a 2D PS colloidal crystal with Au nanoshells into a polyacrylic acid (PAA) hydrogel film. This CAuHCF can act as a visualized sensor with high diffraction intensity. The 2D PS colloidal crystal with Au nanoshells was prepared by depositing an Au layer on PS colloidal crystal obtained by interfacial self-assembly. The diffraction intensity of the CAuHCF was increased by about 30-fold than that of traditional 2D PS colloidal crystal/hydrogel composite film on transparent substrate due to large scattering cross section of Au shell. Such sensors based Au nanoshells array with the simple preparation process and the strong diffraction signal are promising ones for practical applications in visual detection. Additionally, with the simple preparation process and high diffraction intensity, other visualized sensors based different hydrogel matrix and the 2D PS colloidal crystal with Au nanoshells could be synthesized for monitoring various analysts.
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ACS Applied Materials & Interfaces
·
2015
·
IF 6.723
Liangliang Dai,Qingfeng Zhang,Jinghua Li,Xinkun Shen,Caiyun Mu,Kaiyong Cai
In this work, we employed dendrimerlike mesoporous silica nanoparticles with hierarchical pores (HPSNs) to fabricate drug delivery system bioimaging and targeted tumor therapy in vivo. N,N-phenylenebis(salicylideneimine)dicarboxylic acid (Salphdc) was used both as the gatekeeper of HPSNs via pH-responsive coordination bonds between −COOH of Salphdc and In3+ ions and as a fluorescence imaging agent. Folic acid was then conjugated to Salphdc as the targeting unit. The results revealed that the system could deliver model drug DOX to the tumor site with high efficiency and then cause cell apoptosis and tumor growth inhibition. Moreover, the conjugated Salphdc was proved to be a promising fluorescence probe for tracing distribution of the system in vivo. The study affords a potential nanoconainer for cancer therapy and biological imaging.
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BIOMATERIALS
·
2013
·
IF 7.604
Ran Mo,Qiong Sun,Nan Li,Can Zhang
pH-sensitive liposomes (HHG2C 18 -L and PEGHG2C 18 -L) based on zwitterionic oligopeptide lipids as anticancer drug carriers were developed and evaluated for effective intracellular delivery and enhanced antitumor activity . The amino acid-based lipids, 1,5-dioctadecyl- l -glutamyl 2-histidyl-hexahydrobenzoic acid (HHG2C 18 ) and 1,5-distearyl N -( N -α-(4-mPEG2000) butanedione)-histidyl- l -glutamate (PEGHG2C 18 ), were synthesized, which have the multistage pH-response to tumor microenvironmental pH (pH e , pH 6.0–7.0) and endosomal/lysosomal pH (pH i , pH 4.0–6.0) successively. HHG2C 18 -L contains HHG2C 18 , while PEGHG2C 18 -L includes HHG2C 18 and PEGHG2C 18 . Both of them displayed the capability of charge conversion to the surrounding pH. The zeta potentials of HHG2C 18 -L and PEGHG2C 18 -L were negative at pH 7.4, whereas positive at pH 6.5 and more positive at lower pH. Coumarin 6-loaded HHG2C 18 -L (C6/HHG2C 18 -L) and PEGHG2C 18 -L (C6/PEGHG2C 18 -L) showed higher tumor cellular uptake due to electrostatic absorptive endocytosis at pH e (pH 6.5), produced proton sponge effect for endo-lysosomal escape, and accumulated to the mitochondria based on stronger positive charge by the hydrolysis of a pH-sensitive linker at pH i (pH 5.5 and pH 4.5). Furthermore, temsirolimus (CCI-779)-loaded HHG2C 18 -L (CCI-779/HHG2C 18 -L) and PEGHG2C 18 -L (CCI-779/PEGHG2C 18 -L) had significantly higher antiproliferative and apoptosis inducing effects toward the human renal carcinoma (A498) cells at pH 6.5 relative to that at pH 7.4. The half maximal inhibitory concentration (IC50) of CCI-779/HHG2C 18 -L and CCI-779/PEGHG2C 18 -L were about 3 μg/mL and 5 μg/mL at pH 6.5, 1.67-fold and 1.60-fold improved relative to that at pH 7.4, respectively. The total apoptotic ratio of CCI-779/HHG2C 18 -L and CCI-779/PEGHG2C 18 -L increased from 9.90% and 7.78% at pH 7.4 to 19.53% and 12.10% at pH 6.5, respectively. In vivo , CCI-779/PEGHG2C 18 -L after intravenous administration presented remarkably higher bioavailability and blood persistence compared with unPEGylated CCI-779/HHG2C 18 -L, and had the strongest antitumor efficacy against xenograft renal cancer (Renca) tumor models. Accordingly, the results provide the feasibility of using pH-sensitive zwitterionic oligopeptide lipids to extend the applications of liposomes to efficient anticancer drug delivery in cancer therapy.
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2014
·
IF 4.287
Mengtan Cai,Mengtian Leng,Aijing Lu,Liu He,Xiaoxiong Xie,Lei Huang,Yuhao Ma,Jun Cao,Yuanwei Chen,Xianglin Luo
Amphiphilic poly(ɛ-caprolactone)-SS-poly(N,N-diethylaminoethyl methacrylate)-r-poly(N-(3-sulfopropyl)-N-methacrylate-N,N-diethylammonium-betaine) (PCL-SS-PDEASB) was designed and synthesized successfully. pH and redox dually responsive micelles were prepared based on the obtained copolymers, with zwitterionic sulfobetaines as hydrophilic shell, DEA as pH sensitive content and disulfide as redox responsive linkage. The micelle diameters were all less than 200 nm and the micelle diameter distributions were narrow. These micelles could be triggered by pH and redox condition. The drug release from the drug-loaded micelles displayed fastest under simultaneously acidic and reductive conditions. Results of in vitro cell toxicity evaluation showed that introduction of sulfobetaines could greatly decrease the toxicity of poly(ɛ-caprolactone)-SS-poly(N,N-diethylaminoethyl methacrylate) (PCL-SS-PDEA) micelles. DOX-loaded PCL-SS-PDEASB micelles showed higher efficiency to kill HeLa cells than DOX-loaded PCL-PDEASB micelles. Half inhibitory concentration (IC 50 ) of DOX-loaded PCL-SS-PDEASB micelles decreased with the content of sulfobetaines increasing and was even closer to that of DOX·HCl. Thus, the pH and redox dually responsive biodegradable micelles generated by PCL-SS-PDEASB may be potential smart drug carriers for tumor targeted delivery.
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Materials Science & Engineering C-Materials for Biological Applications
·
2014
·
IF 2.736
Juan Huang,Yanan Xue,Ning Cai,Han Zhang,Kaikai Wen,Xiaogang Luo,Sihui Long,Faquan Yu
To reduce leakage on the drug-delivery pathway to minimize side effect of reduction or pH sensitive drug delivery systems, we designed a glutathione (GSH)/pH co-triggered magnetic nanogel drug delivery system for doxorubicin (DOX) based on the GSH concentration and pH difference between intracellular and extracellular environments. The introduction of superparamagnetic iron oxide nanoparticles (SPION) was intended for magnetic targeting. The magnetic DOX-loaded nanogel was then prepared by the oxidation of thiolated alginate with thiolated SPION in the presence of DOX. The nanogel size can be readily regulated in a range of 120–320 nm upon preparation conditions, with a negative surface charge of around − 40 mV. Saturation magnetization was estimated at 27.4 emu/g Fe by VSM. In vitro release was conducted in simulated cancerous environment conditions such as a high GSH concentration and mild acidity. As a result, the nanogel expressed, upon dual stimuli of pH 5/10 mM GSH, significantly higher accumulative release than upon single stimulus of pH 5 without GSH or pH 7.4/10 mM GSH. In vitro cytotoxicity against HeLa cells clearly illustrated that the nanogel could effectively inhibit cell growth, and the IC 50 was figured out to be 2.3 μg/mL of the nanogel, while the nanogel exclusive of DOX was nontoxic. Confocal laser scanning microscopy observation, combined with the result of Prussian blue staining, indicated that DOX was efficiently internalized into HeLa cells through endocytosis, released into the cytoplasm, and then principally entered the nuclei. The quantitative examination of the iron content revealed an exponential increase in the cellular uptake and an exponential decrease in the uptake efficiency with the fed nanogel. This drug-loaded nanogel could be a promising drug carrier for effective tumor-targeted chemotherapy.
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高影响因子
COLLOID AND POLYMER SCIENCE
·
2014
·Vol. 292
·期 5
·1061-1072
·
IF 2.41
Luo Yan-Ling,Yang Xiao-Li,Xu Feng,Chen Ya-Shao,Zhao Xu
pH-sensitive poly(methacrylic acid)- block -hydroxyl-terminated polybutadiene- block -poly(methacrylic acid) block copolymers were synthesized by atom transfer radical polymerization of t -butyl methacrylate and follow-up acidolysis. The copolymers can spontaneously assemble into stable and nearly spherical micelle aggregates in aqueous solution, with hydrodynamic diameters ( D
h
) from 51 to 92 nm and critical micelle concentration of 3.90–7.76 mg L −1 . Z eta potentials were found to be increased with increasing (monomer)/(initiator) molar ratios. A pH-dependent phase behavior is produced at approximately 5.4–5.6, as determined by D
h
and I
335 / I
332 fluorescence intensity ratios. The in vitro camptothecin (CPT) release was compositional and pH dependent, and the cumulative CPT release below pH 7.2 was higher than that in pH 7.4. They could inhibit the premature burst CPT release. The copolymer micelles were low in cytotoxicity even at a micellar concentration of 800 mg L −1 , and therefore they may be used as potential drug-delivery carriers.
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Polymer Chemistry
·
2013
·Vol. 4
·期 15
·4092-4102
·
IF 5.231
Qijing Chen,Xueteng Cao,Hao Liu,Wei Zhou,Lianjie Qin,Zesheng An
Well-defined core cross-linked star (CCS) polymers of poly(N,N-dimethylaminoethyl methacrylate) (PDMAEMA) were prepared via cross-linking copolymerization in an aqueous-based dispersion polymerization system, mediated by reversible addition–fragmentation chain transfer (RAFT) polymerization. The synthesized CCS polymers were characterized by nuclear magnetic resonance (NMR) spectroscopy, gel permeation chromatography (GPC), dynamic light scattering (DLS), and conductivity and zeta potential measurements. The use of PDMAEMA CCS polymers as effective emulsifiers for oil-in-water emulsions was investigated. Interfacial tension measurements showed that the CCS polymer reduced the interfacial tension between water and oil in a pH-dependent manner. Gelled high internal phase emulsions (HIPEs) were formed at high oil fractions (80–89 vol%) and over a wide range of pH values (2–12). The HIPEs were characterized by conductivity, confocal laser scanning microscopy (CLSM) and rheology. The emulsion properties in terms of oil droplet size, long-term stability and rheology were pH-dependent. Complete demulsification of HIPEs was easily realized 2 min after the addition of base. The CCS-stabilized HIPEs were used as templates to prepare porous hydrophilic polymers by polymerizing the monomers in the continuous aqueous phase. The study presented herein reveals that responsive CCS polymers can be used as effective stabilizers for the formation of responsive HIPEs, which have a wide range of applications.
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BIOMACROMOLECULES
·
2013
·
IF 5.371
Yue Huang,Zhaohui Tang,Xuefei Zhang,Haiyang Yu,Hai Sun,Xuan Pang,Xuesi Chen
A series of pH-responsive random copolymer poly(l-glutamic acid-co-l-lysine) [P(Glu-co-Lys)] were synthesized through the ring-opening polymerization (ROP) of γ-benzyl-l-glutamate N-carboxyanhydride (BLG-NCA) and 3-benzyloxycarbonyl-l-lysine N-carboxyanhydride (ZLys-NCA) and the subsequent deprotection. The chemical structure of the P(Glu-co-Lys)s was confirmed by NMR. Critical aggregation concentration and transmission electron microscopy measurements indicated that the P(Glu-co-Lys)s could self-assemble into aggregates in phosphate buffer. The surface charge of P(Glu-co-Lys) aggregates was greatly affected by the solution’s pH and l-glutamic acid/l-lysine ratio because the carboxyl and amino groups present on the P(Glu-co-Lys) aggregates could be protonated or deprotonated to become charged. The pH value of the solution at which the surface charge of the P(Glu-co-Lys) aggregates reversed could be manipulated by the feed ratio of BLG-NCA and ZLys-NCA. In vitro methyl thiazolyl tetrazolium assays demonstrated that negatively charged P(Glu-co-Lys)s were nontoxic and biocompatible. Positive charged P(Glu-co-Lys)s showed some cytotoxicity to Hela cells. Cisplatin (CDDP) was used as a model anticancer drug to evaluate the charge-reversal drug delivery system. By the manipulation of CDDP loading content, the surface charge of the CDDP/P(Glu-co-Lys) nanoparticles could be reversed to positive from negative at tumor extracellular pH (pHe 6.5–7.2). An enhanced drug uptake and inhibition of cancer cell proliferation were observed for the tumoral pHe triggered charge-reversal CDDP/P(Glu-co-Lys) drug delivery system. These indicated that the CDDP/P(Glu-co-Lys) nanoparticles could be used as intelligent drug delivery systems for cancer therapy.
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2014
·Vol. 2014
·期 36
·6156-6164
·
IF 2.965
Liru Cui,Huiming Lin,Chunyu Yang,Xiao Han,Ting Zhang,Fengyu Qu
Graphical A pH-responsive and magnetic-targeted drug-delivery system was prepared with a Fe 3 O 4 @mesoporous silica core–shell nanostructure as host. Au nanoparticles were used as the capping agent. These were connected to the surface of the mesopore through the hydrazone linkage to restrict the drug release. The system has potential applications in low-pH tissue-targeted therapy. A multifunctional nanocomposite has been successfully prepared for pH-responsive and magnetic-targeting drug delivery. First, Fe 3 O 4 @mesoporous silic (mSiO 2 ) core–shell nanoparticles were synthesized as the nanocapsules. Doxorubicin hydrochloride was adopted as the model drug; after drug loading, gold nanoparticles (5 nm) were connected to block the mesopore through the hydrazone linkage. The hydrazone bond, a typical acid-sensitive bond, could undergo hydrolysis in an acidic environment to induce the release of the capping agent, so that the multifunctional nanocomposite revealed acid-enhanced release performance. What's more, before reaching acid conditions, little premature release was found to take place. Cell experiments were also carried out to reveal the good biocompatibility, fast uptake, and improved toxicity toward HeLa cells. Thus, in association with the magnetic target, the multifunctional nanocomposite shows the potential application for some low-pH tissue-targeted therapy, such as for inflammation and tumors.
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BIOMACROMOLECULES
·
2013
·
IF 5.371
Jie Ren,Yanxin Zhang,Ju Zhang,Hongjun Gao,Gan Liu,Rujiang Ma,Yingli An,Deling Kong,Linqi Shi
Herein, a series of biocompatible, robust, pH/sugar-sensitive, core-cross-linked, polyion complex (PIC) micelles based on phenylboronic acid–catechol interaction were developed for protein intracellular delivery. The rationally designed poly(ethylene glycol)-b-poly(glutamic acid-co-glutamicamidophenylboronic acid) (PEG-b-P(Glu-co-GluPBA)) and poly(ethylene glycol)-b-poly(l-lysine-co-ε-3,4-dihydroxyphenylcarboxyl-l-lysine) (PEG-b-P(Lys-co-LysCA)) copolymers were successfully synthesized and self-assembled under neutral aqueous condition to form uniform micelles. These micelles possessed a distinct core-cross-linked core–shell structure comprised of the PEG outer shell and the PGlu/PLys polyion complex core bearing boronate ester cross-linking bonds. The cross-linked micelles displayed superior physiological stabilities compared with their non-cross-linked counterparts while swelling and disassembling in the presence of excess fructose or at endosomal pH. Notably, either negatively or positively charged proteins can be encapsulated into the micelles efficiently under mild conditions. The in vitro release studies showed that the release of protein cargoes under physiological conditions was minimized, while a burst release occurred in response to excess fructose or endosomal pH. The cytotoxicity of micelles was determined by cck-8 assay in HepG2 cells. The cytochrome C loaded micelles could efficiently delivery proteins into HepG2 cells and exhibited enhanced apoptosis ability. Hence, this type of core-cross-linked PIC micelles has opened a new avenue to intracellular protein delivery.
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