LANGMUIR
·
2025
·
IF 3.9
Xiaotong Chen,Yuchen Yang,Yunhui Wen,Shaowei Shi,Weichao Shi
The phase behavior of chiral macromolecules is one of the key subjects in chemistry, biology, and materials science. Here we take poly(L-lactic acid) (PLLA) and mesomeric poly(D, L-lactic acid) (mPLA) mixtures as a model system and investigate the phase separation behaviors in double emulsion droplets. At high mPLA compositions, phase separation creates transient bicontinuous networks or discrete domains at the liquid–liquid interface and eventually generates eyeball-like microcapsules. At low mPLA compositions, phase separation occurs first but is trapped by the lateral crystallization of PLLA, leading to spindle-like microcapsules. The dynamic pathways of phase separation can be further modulated by PLA-based amphiphilic block copolymers, so that microcapsules are configurable between the eyeball-, spindle-, and Janus-like structures. By comparing with phase separation on a plane substrate, we unveil that the phase separation dynamics at the double emulsion interfaces are significantly affected by interfacial properties and hydrodynamic effects. This work clarifies the phase transition dynamics of PLLA/mPLA mixtures at liquid–liquid interfaces and sheds insight into the phase behaviors of chiral macromolecules for their structural modulation.
研究领域:
化学
·
材料科学
·
生物学
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DOI
PubMed
高影响因子
ChemElectroChem
·
2016
·Vol. 3
·期 11
·1781-1786
·
IF 3.506
Xiao Huang,Yaofang Xuan,Lisiqi Xie,Bin Su
Graphical Phase-transfer catalysis : Fe III meso -tetra-(4- N -methyl-pyridyl) porphine (Fe III TMPyP) is found to catalyze oxygen reduction at the liquid/liquid interface. Based on the size-selective ion-transfer voltammetry at the nanoscopic liquid/liquid interface, the reaction is rationalized to proceed through the phase-transfer catalysis mechanism. We report an investigation of the oxygen reduction reaction (ORR) catalyzed by Fe III meso -tetra-(4- N -methyl-pyridyl) porphine (Fe III TMPyP) at the polarized water/1,2-dichloroethane (DCE) interface. Fe III TMPyP is a water soluble pentavalent cation, which has a standard Galvani transfer potential of +0.19 V at the water/DCE interface. By four-electrode cyclic voltammetry and shake-flask biphasic reactions controlled by chemical polarization at the macroscale water/DCE interface, we demonstrated that Fe III TMPyP can catalyze the reduction of O 2 by electron donors (e.g., ferrocene and 1,1′-dimethylferrocene). Further, based on voltammetry at the free-standing silica nanochannel membrane (SNM) supported nano-ITIES (interface between two immiscible electrolyte solutions) array where the transfer of Fe III TMPyP is physically blocked owing to the size-exclusion effect, we proved that the overall reaction proceeds through a phase-transfer catalysis (PTC) process, namely the heterogeneous ion transfer of Fe III TMPyP from water to DCE followed by the homogeneous catalyzed ORR in DCE.
研究领域:
化学
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电化学
·
催化科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Zongbo Zhang,Shiliang Song,Yan Ding,Jianhai Yu,Wenting Wu,Jin Li,Xin Wang,Yong Guo,Liang Gong
The precise and controllable preparation of carbon nanomaterials under mild conditions poses a great challenge, especially for metal-catalysed multiphase preparation. This work proposes an efficient method that utilizing high-density ultrasound to enhance the liquid-liquid interfacial reaction system. Iron-doped carbon dots (Fe-CDs) are successfully synthesized in such a normal temperature and atmospheric-pressure reaction condition. It is shown that transient cavitation provides a high-temperature and high-pressure microenvironment for the preparation of Fe-CDs. Moreover, the size of the reactant droplets is reduced from 200.0 ± 17.3 μm to 8.1 ± 2.9 μm owing to the acoustic flow and cavitation effects, which increases the specific surface area of the two reacting phases and improves the mass transfer coefficient by more than 252.0 %. As a result, the yield increases by more than an order of magnitude (from 0.7 ± 0.1 % to 11.9 ± 0.2 %) and the Fe doping rate reaches 20.9 %. The photocatalytic oxidation conversion of 1,4-Dihydropyridine (1,4-DHP) using the obtained Fe-CDs is as high as 98.2 %. This research gives a new approach for the efficient and safe production of Fe-CDs, which is promising for industrial applications.
研究领域:
材料科学
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化学工程
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环境科学
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产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Peng He,Yi Shao,Zhengyou Yu,Xu Liang,Junjie Liu,Yixuan Bian,Zhiwei Zhu,Meixian Li,Carlos M. Pereira,Yuanhua Shao
Charge (ion and electron)-transfer reactions at a liquid/liquid interface are critical processes in many important biological and chemical systems. An ion-transfer (IT) process is usually very fast, making it difficult to accurately measure its kinetic parameters. Nano-liquid/liquid interfaces supported at nanopipettes are advantageous approaches to study the kinetics of such ultrafast IT processes due to their high mass transport rate. However, correct measurements of IT kinetic parameters at nanointerfaces supported at nanopipettes are inhibited by a lack of knowledge of the nanometer-sized interface geometry, influence of the electric double layer, wall charge polarity, etc. Herein, we propose a new electrochemical characterization equation for nanopipettes and make a suggestion on the shape of a nano-water/1,2-dichloroethane (nano-W/DCE) interface based on the characterization and calculation results. A theoretical model based on the Poisson–Nernst–Planck equation was applied to systematically study how the electric double layer influences the IT process of cations (TMA+, TEA+, TPrA+, ACh+) and anions (ClO4–, SCN–, PF6–, BF4–) at the nano-W/DCE interface. The relationships between the wall charge conditions and distribution of concentration and potential inside the nanopipette revealed that the measured standard rate constant (k0) was enhanced when the polarity of the ionic species was opposite to the pipette wall charge and reduced when the same. This work lays the right foundation to obtain the kinetics at the nano-liquid/liquid interfaces.
研究领域:
电化学
·
生物化学
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Ranying Jiang,Haozhe Yi,Daofan Ma,Taotao Fu,Chunying Zhu,Guangwei Wang,Youguang Ma
The droplet adsorption has many potential applications in microchemical engineering process, vesicle preparation and other various fields. However, the study on adsorption mechanisms and enhancement method remains still scarce so far. The droplet adsorption at the liquid–liquid interface relies primarily on the lubrication pressure in the liquid film, which determines the operating range of adsorption. The interaction between nanoparticles and surfactants distributed in two distinct phases could greatly affect the stability of the liquid film, thereby facilitating the droplet adsorption. In this study, a liquid–liquid–liquid three-phase system is constructed and the enhancement effect of interaction between nanoparticles and surfactants on the droplet interface adsorption process is visually investigated. The influences of the nanoparticle size on the interfacial dynamics and the operating range of droplet adsorption are studied systematically, and the adsorption and enhancement mechanisms are explored. It is found that the electrostatic interaction between PS-COOH NPs and PDMS could promote the rupture of the liquid film. The dense arrangement of nanoparticle-surfactant monolayer at the interface would hinder the evolution of the adsorption interface. Appropriate increase in the size of nanoparticles could facilitate the droplet adsorption process.
研究领域:
微化学工程
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胶体与界面科学
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材料科学
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Mingfu Zhao,Rong Guo,Jia Leng,Shiyu Qin,Jiaxin Huang,Wei Hu,Minggang Zhao,Ye Ma
Microplastics (MPs) pollution has become a focal point of global concern, as the widespread distribution of MPs in the environment poses a potential threat to ecosystems and human health. Despite surface-enhanced Raman scattering (SERS) being one of the most promising detection techniques, the “coffee ring effect” of MPs and their unique size scale make effective contact with SERS substrates challenging. Here, we propose a novel strategy for MPs detection by constructing a plasmonic metasurface at the liquid-liquid interface (LLI). The fluidic properties of LLI provide more flexibility for the uniform dispersion of MPs and the assembly of plasmonic arrays. MPs are captured and assembled on an atomic-level metasurface in a core-shell structure (AuNPs@MPs), providing abundant “hot spots” and additional volume-enhanced Raman effects. This results in enhanced electromagnetic field around MPs and increased enhancement factors, demonstrating high SERS sensitivity and uniformity. This sensing platform provides a new approach for trace detection of MPs and has been validated in practical matrix.
研究领域:
环境科学
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分析化学
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纳米技术
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产品关联
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Haozhe Yi,Taotao Fu,Daofan Ma,Chunying Zhu,Youguang Ma
The droplet transfer across an interface in a microchannel is extensively utilized in diverse fields; however, it is challenging to drive droplets to penetrate the interface at such a small scale. In this study, a novel flow pattern of droplet transfer is observed and the mechanism is investigated; accordingly, an accurate prediction equation for determining the critical condition of droplet transfer is proposed. Meanwhile, the liquid film entrainment is also observed, which leads to the formation of an oil-in-water-in-water system. This study serves as a valuable reference for further studies on the mechanism of droplet transfer and provides practical guidance for its industrial application.
研究领域:
化学工程
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微流控技术
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界面科学
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产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2018
·
IF 3.789
Youchuang Chao,Sze Yi Mak,Qingming Ma,Jing Wu,Zijing Ding,Lei Xu,Ho Cheung Shum
The interfacial phenomena at liquid–liquid interfaces remain the subject of constant fascination in science and technology. Here, we show that fingers forming at the interface of nonequilibrium all-aqueous systems can spontaneously break into an array of droplets. The dynamic formation of droplets at the water–water (w/w) interface is observed when a less dense aqueous phase, for instance, the dextran solution, is placed on a denser aqueous phase, the polyethylene glycol solution, in a vertical Hele-Shaw cell. Because of the gradual diffusion of water from the upper phase into the lower phase, a dense layer appears at the nonequilibrium w/w interface. As a result, a periodic array of fingers emerge and sink. Remarkably, these fingers break up and an array of droplets are emitted from the interface. We characterize the wavelength of fingering by measuring the average distance between the dominant fingers. By varying the initial concentrations of the two nonequilibrium aqueous phases, we identify experimentally a phase diagram with a wide parameter space in which finger breaking occurs. Finally, plenty of droplets, spontaneously formed when one phase is continuously deposited onto another aqueous phase, further confirm the robustness of our experimental results. Our work suggests a simple yet efficient approach with a potential upscalability to generate all-aqueous droplets.
研究领域:
物理学
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材料科学
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流体力学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 56
·期 1
·380-391
·
IF 3.553
Hou Ying,Nie Bei
Abstract With an in situ synthesized AgNO 3 complex molecular cage, icosahedral C 60 can be selectively extracted from fullerene mixture by a facial liquid–liquid interfacial precipitation, resulting in exclusive C 60 organometallic microcrystal (C 60 /C 70 = 6/1). By exploiting its intrinsic insolubility against nonpolar solvent, the C 60 can be separated from the homologues, C 70 , which contrarily is assembled through merely hydrophobic interaction and π-π stacking. The AgNO 3 complex encaged C 60 crystal was morphologically and structurally characterized by SEM, Raman and XRD spectra to revealing the underlying separation mechanism. The selective extraction efficiency (89.7%) was semiquantitatively characterized by combined optical spectroscopy and mass spectrometry, indicating a decent specificity of spontaneously formed molecular cage toward C 60 extraction. Thus, this discovery of a template-specific molecular cavity would pave the way to advance molecular imprinting technology using supramolecular array for fullerene separation, prevailing over the conventional “design-synthesis-performance” strategy by substantially reducing the laborious work and economic cost. Graphic abstract
研究领域:
化学
·
材料科学
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产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2016
·
IF 2.822
Xianhao Zhang,Shudong Zhang,Xin Zhang,Mingzhi Li,Yaxiong Gu,Yuanhua Shao
The electrochemical behaviors of ten derivatives of ketone as the organic phases for the establishment of liquid/liquid interfaces were investigated by cyclic voltammetry and micropipettes. The ionic species limiting the potential window were determined, and relationships between the structure of solvents and the potential window were evaluated. For heptanones and nonanones , the limits of the potential window were affected by the places of carbonyl and the branched structures in carbon chains. We have found that the water/2,6-dimethyl-4-heptanone interface has the widest potential window among these ten ketone derivatives. Simple ion transfers of TPAs + , TBA + , BF 4 − , IO 4 − and ClO 4 − were observed at the water/2,6-dimethyl-4-heptanone interface with BTPPATPBCl and LiCl as the respective organic and aqueous supporting electrolytes , and their thermodynamic data were calculated.
研究领域:
分析化学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Qi Diao,Xiaoyang Li,Mengxiao Diao,Yong-Ill Lee,Hong-Guo Liu
Hypothesis Our previous studies have shown that the metal nanoparticle/polymer composite structures fabricated at the liquid/liquid interface have good reusability but lower catalytic activity for heterogeneous reactions in aqueous solutions. This should be attributed to the poor water wettability and more compact structure of the polymer matrices. Therefore, it should be possible to improve the catalytic activity through designing and fabricating a porous composite structure with good water wettability. Experiments A modified liquid/liquid interface adsorption and fabrication method was used. An aqueous solution of copper acetate and a chloroform/DMF mixed solution of PS- b -PAA acted as the two phases. Through spontaneous emulsification, self-assembly of the polymer molecules with Cu 2+ ions in the droplets, and adsorption of the formed spherical micelles and nanofibers to the planar liquid/liquid interface, a porous composite microstructure was formed. Findings This structure consisted of nanofiber-connected nanospheres which have a PS core and a PAA corona. Tiny and well-dispersed Cu nanoparticles were embedded in the hydrophilic corona and were adsorbed on the nanofibers surface as well. After physical cross-linking with 1,6-diaminohexane, the composite material exhibited high catalytic activity and good reusability for the reactions in aqueous solutions. For example, the rate constant for the reduction of p -nitroaniline reached 1965 s −1 g −1 .
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Zhidan Xu,Yongtao You,Silan Bai,Lishi Wang,Cheng Liu
Antihistamines relieve allergic symptoms by inhibiting the action of histamine. Further understanding of antihistamine transmembrane mechanisms and optimizing the selectivity and real-time monitoring capabilities of drug sensors is necessary. In this study, a micrometer liquid/liquid (L/L) interfacial sensor has served as a biomimetic membrane to investigate the mechanism of interfacial transfer of five antihistamines, i.e., clemastine (CLE), cyproheptadine (CYP), epinastine (EPI), desloratadine (DSL), and cetirizine (CET), and realize the real-time determinations. Cyclic voltammetry (CV) and differential pulse voltammetry (DPV) techniques have been used to uncover the electrochemical transfer behavior of the five antihistamines at the L/L interface. Additionally, finite element simulations (FEMs) have been employed to reveal the thermodynamics and kinetics of the process. Visualization of antihistamine partitioning in two phases at different pH values can be realized by ion partition diagrams (IPDs). The IPDs also reveal the transfer mechanism at the L/L interface and provide effective lipophilicity at different pH values. Real-time determinations of these antihistamines have been achieved through potentiostatic chronoamperometry (I–t), exhibiting good selectivity with the addition of nine common organic or inorganic compounds in living organisms and revealing the potential for in vivo pharmacokinetics. Besides providing a satisfactory surrogate for studying the transmembrane mechanism of antihistamines, this work also sheds light on micro- and nano L/L interfacial sensors for in vivo analysis of pharmacokinetics at a single-cell or single-organelle level.
研究领域:
药理学
·
分析化学
·
生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）