Soft Matter
·
2015
·Vol. 11
·期 20
·4075-4080
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IF 4.029
Lijuan Shi,Fuyu Chen,Nan Sun,Liqiang Zheng
Novel gemini supra-amphiphiles, [Mim-4-Mim][DBS]2 and [Mim-4-Mim][DS]2, were facilely constructed. A slight variation of building blocks can effectively modulate the driving forces for the fabrication of gemini supra-amphiphiles, thus leading to the fine control of subsequent self-assemblies. [Mim-4-Mim][DS]2, constructed via electrostatic attraction, tends to form micelles and hexagonal liquid crystals. Rich lamellar structures, including unilamellar and multilamellar vesicles, planar bilayers, and lamellar liquid crystals can be formed by [Mim-4-Mim][DBS]2, which is constructed through electrostatic and π–π stacking interactions. With increasing temperatures, [Mim-4-Mim][DBS]2 exhibits interesting phase separation in the La phase, behaving like common nonionic surfactants. The cross-linking between vesicles, where the “bola-type” [Mim-4-Mim]2+ cations act as the bridges, was found to promote the elongation of aggregates until the occurrence of phase separation.
研究领域:
材料科学
·
化学
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DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2015
·
IF 2.752
Jiao Wang,Xiao Chen,Wanling Cui,Sijing Yi
pH-responsive vesicles have been prepared from the mixture of 1-(10-(4-formyl-phenoxy) decyl)-pyridinium (FDP) or 1-methyl-3-(10-(4-formyl-phenoxy) decyl) imidazolium (FDI) with 1-octyl amine at a molar ratio of 1:1 in alkaline aqueous solutions. Their structures and morphologies were characterized by transmission electron microscopy with sample preparations by negative staining or freeze-fracture. Basically, the spherical unilamellar vesicles were formed with the mean diameters respectively of about 71 and 107 nm for two supra-amphiphile systems, which were based on the formation of dynamic imine bonds between amine and FDP (i-FDP) or FDI (i-FDI). The loading and release studies of a fluorophore, Nile red (NR), demonstrated the capabilities of these vesicles to encapsulate NR and a rapid release at low pH environment. The vesicles from i-FDP behaved relatively more sensitive to acidic environment than those from i-FDI. The dynamic transitions of supra-amphiphiles were characterized by nuclear magnetic resonance or fluorescence emission spectroscopy measurements. A lower critical micelle concentration and a higher aldehyde conversion efficiency of i-FDI than those of i-FDP were observed. The characteristics of facile formation, fast dissociation, and switchable morphologies of studied systems should be referable for designing novel smart supra-amphiphile systems with potential applications as controlled drug delivery systems.
研究领域:
生物化学
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材料科学
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药物递送
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DOI
高影响因子
Soft Matter
·
2018
·Vol. 14
·期 11
·2112-2117
·
IF 3.709
Shangyang Li,Aiyou Hao,Jian Shen,Ningzhao Shang,Chun Wang
In order to fabricate a novel supra-amphiphile with multiple stimulus properties, we developed the strategy of introducing a bi-functional linker to bridge the hydrophilic and hydrophobic building blocks together, by utilizing more than one kind of interaction. We characterized the assembled structure and morphology of the supra-amphiphile using transmission electron microscopy (TEM), dynamic light scattering (DLS) and X-ray diffraction (XRD). 1H NMR and UV-vis spectroscopy studies revealed that the amphiphile was constructed by the effect of host–guest recognition and a dynamic covalent bond, which could be switched ‘‘on’’ and ‘‘off’’ via UV irradiation and pH variation stimuli, respectively. This responsiveness realized finely controllable self-assembly behaviors of the supra-amphiphile, which was thus able to encapsulate and release the drug model rhodamine B.
研究领域:
材料科学
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化学
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生物医学工程
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DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 57
·52189-52200
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IF 3.289
Tao Sun,Lan Shu,Jian Shen,Chunhui Ruan,Zhifeng Zhao,Chen Jiang
Superamphiphiles are considered as a promising approach for fabricating stimuli-responsive materials. Sensitivity to more than one stimulus can improve the system's versatile performance. In this study, we proposed a facile dual-responsive vesicle constructed from Bola-type superamphiphiles. An azobenzene dimer linked by a disulfide bond was synthesized. As the guest molecule, the azobenzene dimer can be included into the β-cyclodextrin's cavity from both ends to form a novel Bola-type superamphiphile, which can further assemble into a vesicular structure in aqueous solution. The vesicles were characterized by transmission electron microscopy (TEM) and dynamic light scattering (DLS). The formation mechanism of the vesicular structure was suggested based on the NMR, Fourier transform infrared spectroscopy (FT-IR) and X-ray diffraction (XRD) results. The photo and redox responsiveness of the vesicles was studied. The vesicles were found able to carry mitomycin C (MMC) and the drug-release can be greatly promoted upon UV irradiation or reduction.
研究领域:
材料科学
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生物化学
·
药学
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DOI
高影响因子
LANGMUIR
·
2021
·
IF 3.882
Qi Hao,Yuetong Kang,Jiang-Fei Xu,Xi Zhang
A novel fluorescence “turn-on” enzyme-responsive supra-amphiphile is developed based on the host–guest recognition between γ-cyclodextrin (γ-CD) and an amphiphilic tetraphenylethene-sodium glycyrrhetinate conjugate (TPE-SGA). The covalent amphiphile TPE-SGA displayed strong fluorescence in aqueous solution owing to the aggregation-induced emission. Upon addition of γ-CD, the fluorescence of TPE-SGA was effectively turned off due to the host–guest recognition with γ-CD prohibiting the aggregation of TPE-SGA in aqueous solution. The as-formed nonfluorescent supra-amphiphile (TPE-SGA/γ-CD) inherited the α-amylase-responsive property of γ-CD. In the presence of α-amylase, the fluorescence of the supra-amphiphile was gradually turned on owing to the hydrolysis of γ-CD, and the fluorescence intensity linearly correlated to the activity of α-amylase. This study enriches the field of supra-amphiphile on the basis of cyclodextrin-based host–guest chemistry and provides a novel strategy to construct fluorescence turn-on functioned self-assemblies. It is anticipated that the fluorescence turn-on supra-amphiphile has potential applications in biological analysis and diagnosis of pancreatic diseases.
研究领域:
超分子化学
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生物分析
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医学诊断
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DOI
高影响因子
Soft Matter
·
2015
·Vol. 12
·期 4
·1192-1199
·
IF 4.029
Huixin Zou,Hongcheng Sun,Liang Wang,Linlu Zhao,Jiaxi Li,Zeyuan Dong,Quan Luo,Jiayun Xu,Junqiu Liu
Glutathione peroxidase (GPx) is a major defense against hydroperoxides as a kind of seleno-enzyme that protects cells from oxidative damage. A supramolecular vesicle with controllable GPx activity and morphology has been successfully constructed by the self-assembly of supra-amphiphiles formed by host–guest recognition between cyclodextrin and adamantane derivatives. By introducing thermosensitive poly(N-isopropylacrylamide) (PNIPAM) scaffolds and the catalytic moiety selenium into adamantane and cyclodextrin, respectively, the complex of catalysis-functionalized cyclodextrin with thermosensitivity-functionalized adamantane directed the formation of a supramolecular vesicle which acted as a GPx mimic at 37 °C. The self-assembled nanoenzyme exhibited an obvious temperature responsive characteristic and high GPx-like catalytic activity promoting the reduction of hydrogen peroxide (H2O2) with glutathione (GSH) as the reducing substrate at 37 °C. However, the vesicle disassembled when the temperature decreased to 25 °C due to the transition of PNIPAM between the coil and the globule. Interestingly, the catalytic activity changed along with the transformation of morphologies. The vesicle structure self-assembled at 37 °C provided the favorable microenvironment for the enzymatic reaction, hence we successfully developed a temperature-responsive nanoenzyme model. Moreover, the catalytic activity of the thermosensitive GPx mimic exhibited excellent reversibility and typical saturation kinetics behaviour similar to a natural enzyme catalyst. It is assumed that the proposed GPx model not only has remarkable advantages such as easy functionalization and facile preparation but also provided a new way to develop intelligent responsive materials.
研究领域:
生物化学
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材料科学
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仿生学
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DOI
PubMed
高影响因子
JOURNAL OF SURFACTANTS AND DETERGENTS
·
2018
·Vol. 22
·期 2
·209-216
·
IF 1.454
Jun Li,Hui Li,Jie Wang,Hongshi Jiang,Chenzhong Yao,Gaofeng Wang,Huixuan Ma,Lijuan Shi
A new kind of trimeric supra-amphiphile [M-4-M-4-M][DBS] 3 that exhibits diverse self-assembly behaviours was fabricated through ion exchange between linear tricationic imidazolium chloride ([M-4-M-4-M]Cl 3 ) and sodium dodecyl benzene sulfonate (SDBS). Micelles are spontaneously transformed into unilamellar vesicles at a quite low concentration (1.5 mM), and then evolved to multilamellar vesicles and planar bilayers successively with a further increase in the concentration of [M-4-M-4-M][DBS] 3 in the absence of any additives. The presence of π-π stacking interactions has been proved to promote the lamellar arrangement of the supra-amphiphile. With increasing temperatures, [M-4-M-4-M][DBS] 3 exhibits interesting “clouding” and phase separation in the L a phase, behaving like common nonionic surfactants. Chain-like aggregates are formed in the bottom phase, which are probably induced by the hierarchical assembly of vesicles. This work provides useful insights into the role of weak interactions in the fabrication and self-assembly of oligomeric supra-amphiphiles, and paves a way to enrich the structures and functions of self-assemblies.
研究领域:
化学
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材料科学
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生物学
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DOI
高影响因子
Soft Matter
·
2016
·Vol. 12
·期 42
·8682-8689
·
IF 3.798
Lijuan Shi,Panpan Sun,Liqiang Zheng
Gemini supra-amphiphiles with different spacer lengths, [M-n-M]2+@2[DBS]− (n = 2, 6, 10), were easily constructed. The conformational flexibility and hydrophobicity of the spacer group can be effectively tailored through regulating the spacer length, leading to the fine control of the topologies and subsequent hierarchical self-assemblies of [M-n-M]2+@2[DBS]−. Vesicles are primarily fabricated by [M-n-M]2+@2[DBS]−, and then successively fused into vesicle clusters, nanotubes, and planar bilayers, whose bilayer curvatures are gradually decreased, with increasing spacer length. Coating [M-10-M]2+ with β-CD can reduce the flexibility and hydrophobicity of the decyl spacer, resulting in the reversion from planar bilayers to vesicles. Furthermore, stable aqueous two-phase systems (ATPSs) that spontaneously formed via vesicle fusion in the solutions of [M-n-M]2+@2[DBS]− (n = 6, 10) can act as functional supramolecular systems in the isolation and purification of oil-soluble biomaterials.
研究领域:
化学
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材料科学
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生物学
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DOI
PubMed
高影响因子
LANGMUIR
·
2023
·
IF 3.9
Zhen Zhao,Lu Zhang,Hao Zhang,Guoqiang Lu,Tong Meng,Hongguo Hao,Yongmin Zhang,Jun Li,Hui Yan
The superamphiphiles exhibit broad prospects for fabricating stimuli-responsive emulsions. Because the superamphiphiles are assembled via noncovalent interactions, they have the advantage of fast response and high efficiency. Recently, a series of switchable emulsions using CO2-responsive superamphiphiles have been developed, which extends the applications of CO2-responsive materials in widespread field. However, there is still a lack of fundamental understanding on the switching mechanism related to the assembled structure of superamphiphiles at the oil–water interface. We employed molecular dynamics (MD) simulations to investigate the reversible emulsification/demulsification process of a responsive emulsion system stabilized by a recently developed responsive superamphiphile (BTOA), which consists of oleic acid (OA) and cationic amine (named 1,3-bis(aminopropyl)tetramethyldisiloxane, BT). The simulation results present the morphologies in both the emulsion and demulsification states. It is found that the ionized OA– and the protonated BT+ together form an adsorption layer at the oil–water interface. The hydrophobic parts of BT+ are inserted into the adsorption layer, and the two amine groups contact the water phase. This adsorption layer reduces the interfacial tension and stabilizes the emulsion. After the bubbling of CO2, the surfactants were fully protonated to OA and BT2+. Because of the changes in the molecular polarity, OA and BT2+ entered the oil and water phases, respectively, resulting in demulsification. The structural and dynamical properties were analyzed to reveal the different intermolecular interactions that were responsible for the reversible reversibility of the emulsion. The observations are considered to be complementary to experimental studies and are expected to provide deeper insights into studies on developing responsive materials via supramolecular assemblies.
研究领域:
化学
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材料科学
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计算科学
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DOI
PubMed
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Zhenghao Zhang,Bo Peng,Yupeng Zhang,Jiaxin Xiong,Jingwei Li,Jianwei Liu
A CO2/N2-responsive emulsion provides milder reaction conditions, nontoxicity, and economic feasibility compared to other switchable surfactants. In this study, CO2/N2-responsive pickering emulsions were fabricated by using a compounded dispersion containing SiO2 nanoparticles (NPs) and superamphiphiles as the emulsifying agents. The synergistic effects of the SiO2 NPs and superamphiphiles significantly stabilized the emulsion at all of the tested concentrations and prevented complete phase separation of oil and water. The electrostatic interaction between the SiO2 NPs and superamphiphiles was disrupted after bubbling with CO2 for 30 s, resulting in the breaking of the emulsion. However, the dispersion recovered its interfacial activity after the introduction of N2 and again emulsified the emulsion. This reversible switching behavior was validated through three consecutive cycles of bubbling CO2/N2. The protonation and deprotonation of the SiO2 NPs and superamphiphiles in response to CO2/N2 facilitated reversible assembly and disassembly, which enabled the switching of the emulsions between inactive and active forms. The novel highly stable Pickering emulsions demonstrated rapid demulsification and emulsification in response to CO2/N2 and are promising for a wide range of applications.
研究领域:
材料科学
·
化学工程
·
胶体与界面科学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Shujuan Yang,Keyang Mai,Congying Xu,Furui He,Qingmei Zhu,Haifang Liu,Gaobo Yu,Yuhong Feng,Jiacheng Li
In view of the micro/nanostructure tunability of colloid particles, they acted as agrichemical delivery systems. Herein, supra-amphiphilic colloids were fabricated using a host–guest interfacial recognition-architected emulsion template strategy and controlled their agricultural interfacial interactions with the superhydrophobic target surface. Interestingly, the supramolecular interfacial system possessed redox-stimulated molecular reconfigurability by regulating aggregation/disaggregation behaviors. Therefore, the surface roughness of silver willow-like supramolecular colloids was readily modulated by tuning the micro/nanointerfaces of the emulsion template, which exhibited a topology and pliability that allowed them to adapt to the micro/nanostructures of leaf surfaces. It simultaneously solved comprehensive problems of adhesion, bounding, and rainwashing of pesticide droplets by the multiscale coupling effect. Intriguingly, the pesticide retention dominantly depended on the degree of surface roughness of silver willow-like supramolecular colloids, and the most roughened one showed greatest in vitro antifungal efficiency against Botrytis cinerea, reaching 91.8% even through multiple rainwashing. Results disclosed that the supra-amphiphilic colloids addressed the entire application processes for promoting the development of sustainable agricultural science.
研究领域:
农业科学
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材料科学
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化学工程
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环境科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xinyu Zhao,Qu Zeng,Shujuan Yang,Furui He,Wenqi Qin,Zhaojun Wang,Keyang Mai,Gaobo Yu,Junhao Huang,Jiacheng Li,Yuhong Feng
Encouraged by the strategy of increasing efficiency and reducing pesticide overuse, the development of polymer/surfactant as additives to enhance pesticide droplet deposition on hydrophobic leave is a promising project. Herein, Alginate-based supra-amphiphiles (SAs), host–guest self-assembled by host amphiphilic cyclodextrin-functionalized alginate derivative (Alg-CD) and guest azobenzene-based surfactant (Azo-DEMA), performed comprehensive characteristics, which integrated the viscosity effect and the ability to reduce surface tension. SAs enabled oil-in-water pesticide droplets to inhibit splashing and light-regulate wetting, thereby enhancing droplets deposition. By analyzing the impact dynamics of loaded-pesticide o/w droplets on hydrophobic surface, the addition of SAs rapidly afforded the pinning ability of droplets with the target surface, and in turn, resulted in inhibiting splashing. Afterward being exposed to UV light, the resulting SAs o/w droplets undergone disassembly so as to release small-molecular surfactant and reduce the surface tension of droplets for improving droplets’ wettability. Importantly, quartz crystal microbalance with dissipation monitoring (QCM-D) was skillfully used for revealing the interaction mechanism between droplets and the waxy layer of hydrophobic surface, finding that SAs could form compact conformation on the waxy surface, while disassembled SAs undergoing UV irradiation exhibited the large adsorption amount and stronger interaction with waxy layer. Consequently, the herbicidal activity experiments exhibit sensitive pesticide control effects assessed under UV even natural sunlight. Light-regulating host–guest interfacial interaction of polysaccharide-based supra-amphiphiles may provide a novel, eco-friendly and feasible manner for comprehensive pesticide applications.
研究领域:
材料科学
·
化学
·
农业科学
·
环境科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）