Soft Matter
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2017
·Vol. 13
·期 35
·5888-5896
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IF 3.889
Handi Yin,Peizhu Zheng,Jihua Zhao,Weiguo Shen
The heats of mixing for a series of DTAB/TX100 mixed surfactant aqueous solutions were measured by flow-mixing calorimetry and isothermal titration calorimetry (ITC) at 298.15 K and 85 kPa, which were used to calculate the inter-micellar interaction enthalpies (−ΔHC). The signs of −ΔHC for pure DTAB and TX100 micellar systems were contrary to the inter-micellar interaction parameters reported for the same systems in the literature, suggesting that these interaction parameters might have a Gibbs free energy character dominated by entropy changes. It was found that the inter-micellar interaction enthalpies varied with the total surfactant concentration and the mixed ratio of the two surfactants, and characterized different structures of the mixed micelles. These phenomena were discussed based on the effects of structural water around the micellar interface, the hydration of counterions, and the repulsive Coulombic interaction.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2016
·
IF 2.76
Junhao Huang,Shixin Zhang,Yuhong Feng,Jiacheng Li,Huiqiong Yan,Furui He,Guizhen Wang,Yanfeng Liu,Lining Wang
A pH-responsive anionic wormlike micellar (WLM) system formed by sodium oleate (NaOA) and benzyltrimethyl ammonium bromide were studied via rheological measurements and dynamic light scattering measurements. The anionic WLMs were used as templates to synthesize mesoporous silicas (MSs). The microstructures of the WLM system can be controlled by altering the pH. The transformation between NaOA and oleic acid changes the charges on the micelle surface and affects the viscoelasticity of the system. High NaOA concentration increases the activation energy (E a ) of the system, whereas a high pH value promotes the formation of spherical micelles and reduces the E a of the solutions. By contrast, a low pH value increases the viscosity of the system given that the electrostatic repulsion between NaOA head-groups is weakened. However, if numerous NaOAs transform into insoluble oleic acids, the viscosity of the system will dramatically decrease. In addition, micelle length and NaOA concentration affect the microstructure of MSs.
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RSC Advances
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2016
·Vol. 6
·期 25
·20761-20771
·
IF 3.289
Weiwei Zhang,Delong Zhang,Xiaoshan Fan,Guangyue Bai,Yuming guo,Zhiguo Hu
Four new Y-shaped miktoarm amphiphilic copolymers were synthesized by ring-opening polymerization (ROP) and click chemistry. The structure of these copolymers was determined by nuclear magnetic resonance (NMR), Fourier transform infrared spectroscopy (FT-IR) and gel permeation chromatography (GPC). The stereocomplexes were prepared by an evaporation method and confirmed by FT-IR, differential scanning calorimetry (DSC) and X-ray diffraction (XRD). Further the aggregation behaviors of these synthesized polymers and their stereocomplexes were studied by fluorescence spectroscopy (PL), transmission electron microscopy (TEM) and light scattering (LS). Their critical micelle concentrations (CMC) obtained by PL were 0.005 mg mL−1 for MPEG1.9k–(scPLA4.5k)2 and 0.039 mg mL−1 for MPEG5k–(scPLA4.5k)2. The aggregation morphologies of homochiral copolymers were worm-like aggregates, while for the stereocomplexes, the spherical micelles were visually observed. The biocompatibility of these copolymers and their stereocomplexes was evaluated with relatively lower cytotoxicity. Finally, the release of doxorubicin (DOX) encapsulated into the micelles in buffer at pH 5.4 was faster than that at pH 7.4. This study demonstrates that the DOX-loaded stereocomplex micelles could be a potential carrier for cancer treatments.
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ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Lei Ye,Yabin Zhang,Boguang Yang,Xin Zhou,Junjie Li,Zhihui Qin,Dianyu Dong,Yuanlu Cui,Fanglian Yao
Over the last few decades, nanoparticles have been emerging as useful means to improve the therapeutic efficacy of drug delivery and medical diagnoses. However, the heterogeneity and complexity of blood as a medium is a fundamental problem; large amounts of protein can be adsorbed onto the surface of nanoparticles and cause their rapid clearance before reaching their target sites, resulting in the failure of drug delivery. To overcome this challenge, we present a rationally designed starch derivative (SB-ST-OC) with both a superhydrophilic moiety of zwitterionic sulfobetaine (SB) and a hydrophobic segment of octane (OC) as functional groups, which can self-assemble into “stealth” micelles (SSO micelles). The superhydrophilic SB kept the micelles stable against aggregation in complex media and imbued them with “stealth” properties, eventually extending their circulation time in blood. In stability and hemolysis tests the SSO micelles showed excellent protein resistance properties and hemocompatibility. Moreover, a phagocytosis test and cytokine secretion assay confirmed that the SSO micelles had less potential to trigger the activation of macrophages and were more suitable as a drug delivery candidate in vivo. On the basis of these results, doxorubicin (DOX), a hydrophobic drug, was used to investigate the potential application of this novel starch derivative in vivo. The results of the pharmacokinetic study showed that the values of the plasma area under the concentration curve (AUC) and elimination half-life (T1/2) of the SSO micelles were higher than those of micelles without SB modifications. In conclusion, the combination of excellent protein resistance, lower macrophage activation, and longer circulation time in vivo makes this synthesized novel starch derivative a promising candidate as a hydrophobic drug carrier for long-term circulation in vivo.
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Acta Biomaterialia
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2016
·
IF 6.008
Zhen-Gang Ma,Rui Ma,Xiao-Lin Xiao,Yong-Hui Zhang,Xin-Zi Zhang,Nan Hu,Jin-Lai Gao,Yu-Feng Zheng,De-Li Dong,Zhi-Jie Sun
Colon-targeted drug delivery and circumventing drug resistance are extremely important for colon cancer chemotherapy. Our previous work found that dimethyl fumarate (DMF), the approved drug by the FDA for the treatment of multiple sclerosis, exhibited anti-tumor activity on colon cancer cells. Based on the pharmacological properties of DMF and azo bond in olsalazine chemical structure , we designed azo polymeric micelles for colon-targeted dimethyl fumarate delivery for colon cancer therapy. We synthesized the star-shape amphiphilic polymer with azo bond and fabricated the DMF-loaded azo polymeric micelles. The four-arm polymer star-PCL-azo-mPEG (sPCEG-azo) (constituted by star-shape PCL (polycaprolactone) and mPEG (methoxypolyethylene glycols)-olsalazine) showed self-assembly ability. The average diameter and polydispersity index of the DMF-loaded sPCEG-azo polymeric micelles were 153.6 nm and 0.195, respectively. In vitro drug release study showed that the cumulative release of DMF from the DMF-loaded sPCEG-azo polymeric micelles was no more than 20% in rat gastric fluid within 10 h, whereas in the rat colonic fluids, the cumulative release of DMF reached 60% in the initial 2 h and 100% within 10 h, indicating that the DMF-loaded sPCEG-azo polymeric micelles had excellent colon-targeted property. The DMF-loaded sPCEG-azo polymeric micelles had no significant cytotoxicity on colon cancer cells in phosphate buffered solution (PBS) and rat gastric fluid. In rat colonic fluid, the micelles showed significant cytotoxic effect on colon cancer cells. The blank sPCEG-azo polymeric micelles (without DMF) showed no cytotoxic effect on colon cancer cells in rat colonic fluids. In conclusion, the DMF-loaded sPCEG-azo polymeric micelles show colon-targeted DMF release and anti-tumor activity, providing a novel approach potential for colon cancer therapy. Statement of Significance Colon-targeted drug delivery and circumventing drug resistance are extremely important for colon cancer chemotherapy. Our previous work found that dimethyl fumarate (DMF), the approved drug by the FDA for the treatment of multiple sclerosis, exhibited anti-tumor activities on colon cancer cells ( Br J Pharmacol . 2015 172 ( 15 ): 3929-43 .). Based on the pharmacological properties of DMF and azo bond in olsalazine chemical structure, we designed azo polymeric micelles for colon-targeted dimethyl fumarate delivery for colon cancer therapy. We found that the DMF-loaded sPCEG-azo polymeric micelles showed colon-targeted DMF release and anti-tumor activities, providing a novel approach potential for colon cancer therapy.
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ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Yufen Li,Yuanna Sun,Ying Xiao,Guorong Gao,Shuhui Liu,Jianfeng Zhang,Jun Fu
Multiresponsive polyelectrolyte hydrogels with extraordinary toughness have great potential in soft device applications. Previously we have demonstrated a series of tough and multiresponsive hydrogels by using multifunctional triblock copolymer (Pluronic F127 diacrylate, F127DA) micelles to cross-link cationic polyelectrolyte chains into 3D network. Herein, we further synthesize negatively charged hydrogels comprising 2-acrylamido-2-methyl propylsulfonic acid (AMPS) monomers by using F127DA micelles as cross-linkers. Similar to the positive nanomicelle (NM) hydrogels, the negative NM hydrogels exhibited a compressive strength up to 59 MPa with a fracture strain up to 98%, and tensile fracture strain higher than 2000%. These charged hydrogels were actuated by electric field when immersed in salt solutions. The effects of electrolyte concentration, electric field strength, and ionic monomer content on the electric actuation behavior of these electroactive hydrogels (EAHs) have been systematically investigated. It is concluded that the electroactive hydrogels show a fast actuation rate with a bending angle up to 87° at 120 s and the bending angle was cyclically reversed upon changing bias direction without a large decrease. This study demonstrates that such tough and multiresponsive electroactive hydrogels may have great potential in sensors, actuators, switches, and artificial muscles.
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COLLOID AND POLYMER SCIENCE
·
2017
·Vol. 295
·期 2
·371-378
·
IF 1.723
Wang Youpeng,Li Guo,Cheng Ruidong,Zhang Xuan,Jiang Jinqiang
Amphiphilic random copolymer micelle of P(NVP- co -NHPM) that responds to both UV and NIR light was designed and investigated. N -hydroxyphthalimide methacrylate — bearing a photoacid generator functional group was synthesized and used to construct the hydrophobic segment of P(NVP- co -NHPM); the N–O bond can be photocleaved when exposing the polymer aqueous solution to 310 nm UV light irradiation, inducing the micellar dissociation and delivery of loaded substances. Dynamic light scattering (DLS), atomic force microscope (AFM), and transmission electron microscopy (TEM) were used to characterize the micellar dissociation and controlled release processes. Moreover, the upconverting nanoparticles (NaLuF 4 :Gd/Yb/Tm) that can effectively absorb NIR light and convert it into visible and UV light were coloaded into polymer micelles to activate the micellar dissociation and the delivery of loaded cargoes via 980 nm NIR light.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2017
·
IF 3.887
Yuling Su,Lili Zhao,Fancui Meng,Quanxin Wang,Yongchao Yao,Jianbin Luo
In order to improve the antibacterial activities while decrease the cytotoxity of silver nanoparticles, we prepared a novel nanocomposites composed of silver nanoparticles decorated lipase-sensitive polyurethane micelles (PUM-Ag) with MPEG brush on the surface. The nanocomposite was characterized by UV–vis, TEM and DLS. UV–vis and TEM demonstrated the formation of silver nanoparticles on PU micelles and the nanoassembly remained intact without the presence of lipase. The silver nanoparticles were protected by the polymer matrix and PEG brush which show good cytocompatibility to HUVEC cells and low hemolysis. Moreover, at the presence of lipase, the polymer matrix of nanocomposites is subject to degradation and the small silver nanoparticles were released as is shown by DLS and TEM. The MIC and MBC studies showed an enhanced toxicity of the nanocomposites to both gram negative and gram positive bacteria, i.e. E. coli and S. aureus , as the result of the degradation of polymer matrix by bacterial lipase. Therefore, the nanocomposites are biocompatible to mammalian cells cells which can also lead to activated smaller silver nanoparticles release at the presence of bacteria and subsequently enhanced inhibition of bacteria growth. The satisfactory selectivity for bacteria compared to HUVEC and RBCs make PUM-Ag a promising antibacterial nanomedicine in biomedical field.
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RSC Advances
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2016
·Vol. 6
·期 84
·80896-80904
·
IF 3.289
Hongliang Cao,Huajie Song,Debiao Xie,Chao Chen,Xin Chen,Ping Wang,Wenxin Wang
We report a glutathione (GSH) responsive drug carrier that is based on the Michael addition reaction between an olefinic bond and GSH. Amphiphilic copolymers with multi-linear-cyclized and branched structures that contain vinyl groups were successfully synthesized by deactivation enhanced atom transfer radical polymerization (DE-ATRP). The polymers self-assembled into GSH responsive micelles with sizes of 68 to 97 nm and spherical morphology. The core cross-linked micelles were confirmed to greatly decrease doxorubicin (DOX) leakage due to the concentration gradient. Drug release experiments indicated that the drug carrier containing no disulfide has the same responsive ability as a conventional GSH reduction responsive carrier with a similar polymer structure. MTT assays showed that the blank micelles are totally non-cytotoxic, while the DOX-loaded micelles exhibit GSH-dependent behaviour.
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MACROMOLECULAR BIOSCIENCE
·
2016
·Vol. 17
·期 3
·1600258
·
IF 3.68
Shan Zhang,Jianbin Xu,Heng Chen,Zhangfa Song,Yalan Wu,Xingyi Dai,Jie Kong
In this contribution, amphiphilic star copolymers (H40- star -PCL- a -PEG) with an H40 hyperbranched polyester core and poly(ε-caprolactone)- a -poly(ethylene glycol) copolymer arms linked with acetal groups are synthesized using ring-opening polymerization and a copper (I)-catalyzed alkyne-azide cycloaddition click reaction. The acid-cleavable acetal groups between the hydrophilic and hydrophobic segments of the arms endow the amphiphilic star copolymers with pH responsiveness. In aqueous solution, unimolecular micelles can be formed with good stability and a unique acid degradability, as is desirable for anticancer drug carriers. For the model drug of doxorubicin, the in vitro release behavior, intracellular release, and inhibition of proliferation of HeLa cells show that the acid-cleavable unimolecular micelles with anticancer activity can be dissociated in an acidic environment and efficiently internalized by HeLa cells. Due to the acid-cleavable and biodegradable nature, unimolecular micelles from amphiphilic star copolymers are promising for applications in intracellular drug delivery for cancer chemotherapy.
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ACS Applied Nano Materials
·
2025
·
IF 5.5
Su-Yu Yang,Shu-Tong Li,Tian-Hua Li,De-Jin Ma,Jun-Jie Yu,Yang Liu,Yang Yu,Xue-Tao Li,Juan Zang,Zi-Min Yuan,Liang Kong
Hepatocellular carcinoma (HCC) represents a significant health challenge that requires urgent attention, primarily due to the limited application of chemotherapeutic drugs. This limitation arises from the high infiltration of immune cells within the tumor microenvironment, which diminishes the effectiveness of the therapeutic agents. Consequently, exploring the combination of drug therapy with the M1 polarization mechanism is considered a promising strategy to address this issue. In this study, we designed a hierarchically targeted micelle system responsive to reactive oxygen species (ROS), enabling the synergistic delivery of the hydrophobic drugs sorafenib (Sof) and dehydrodiisoeugenol (Deh) through the integration of a ROS-sensitive bond (thioacetal ketones, TK) and a specific targeting group (glycyrrhetinic acid, GA). The results demonstrated that TK-GA-Sof/Deh-Ms exhibited excellent encapsulation efficiency and stability. The cumulative release rates of Sof and Deh from TK-GA-Sof/Deh-Ms at 48 h were recorded as 49.67 ± 0.02% and 43.90 ± 0.01%, respectively. The online SynergyFinder2.0 software was used to calculate a ZIP synergy score of 6.339 for Sof and Deh, indicating synergy. The combination showed a more significant antitumor effect. The IC50 value of TK-GA-Sof/Deh-Ms was 13.21 ± 1.36 μM. Notably, Deh not only promotes the polarization of M1 macrophages but also effectively inhibits the activation of M2 macrophages. In summary, this study introduces a stepwise-targeting micelle system for liver cancer that possesses dual functions─tumor inhibition and macrophage regulation, thereby paving the way for innovative treatment strategies for hepatocellular carcinoma.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Xiaowei Tan,Ziyi Liu,Cuiling Ouyang,Minxin Deng,Jingyi Xiao,Shufen Xiao,Tuo Huang,Siyu Yu,Hezhang Chen,Hui Chu,Jian Chen
Chitosan (CS)-based drug delivery systems often face challenges in obtaining clinical approval. Enhancing the binding affinity of CS-based carriers to target cells, such as tumor cells, is crucial for their translation from bench to bedside. Strategies like crosslinking (NHS-disulfide-NHS) and utilizing materials like albumin have proven effective in strengthening interactions between CS-based nanoparticles and tumor cells, thereby enhancing cellular uptake (cellular avidity). This study presents a novel approach using crosslinked CS nanoparticles loaded with doxorubicin, featuring reduction-responsive drug release and albumin coating. The albumin-coated crosslinked chitosan (ACCC) was assembled via reaction between amino of CS/albumin and NHS-disulfide-NHS. The resulting ACCC nanoparticle micelles demonstrate enhanced stability of the micelles. The hybrid crosslinked network ensures stability while providing ample space for drug loading and achieves reduction-responsive drug release through disulfide bond crosslinking. Moreover, the proposed system possesses excellent biocompatibility. Compared to uncoated crosslinked chitosan nanoparticle micelles, ACCC nanoparticle micelles exhibit potent cytotoxicity against tumor cells, particularly in reducing environment. Fluorescence imaging and flow cytometry analyses confirm the enhanced cellular affinity conferred by albumin coating. These findings underscore the potential of ACCC nanoparticles in improving tumor cell adhesion and anti-tumor efficacy, thus offering promising prospects for translational medicine in CS-based drug delivery.
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