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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2024 · IF 10.8

Tailoring Polyelectrolyte Multilayer Nanofiltration Membranes by Aerosol-Assisted Printing: Insights into Membrane Formation Mechanisms

Lihong Gan,Jin Zhang,Yangtao Wu,Zhuo Chen,Zhenyu Zhao,Shihong Lin,Yi Jiang

Polyelectrolyte multilayer (PEM) membranes, with advantageous features of versatile chemistry and structures, are driving the development of advanced nanofiltration (NF) membranes with exceptional performance. While developing a printing method holds great promise for the eventual mass production of these membranes, reports on the printing method and the underlying mechanisms of membrane formation are currently scarce. Herein, we develop an aerosol-assisted printing (AAP) system for fabricating PEM NF membranes with highly tunable separation characteristics. Our study unveils the three stages of membrane formation from assembly of polyethylenimine (PEI) and poly(sodium 4-styrenesulfonate) (PSS): aerosol deposition, single PE layer formation, and PEM assembly. The droplet deposition is governed by inertial impaction, and the deposited PEs migrate/entangle to form a single PE layer. The thicknesses of the PE layer and PEM exhibit linear growth as the number of printing scan increases. Furthermore, PE interdigitation forms an effective polymeric network barrier, which increases the resistance to solute and water transport. By manipulating the PE deposition mass and layering, PEM membranes with tunable pore radii (0.40–0.56 nm) and water permeability (5–60 L·m–2·h–1·bar–1) were obtained for various water treatment applications, ranging from micropollutant removal to humic acid filtration. Our study offers valuable mechanistic insights into the PEM formation and precise structural adjustment via printing, thus facilitating scalable manufacturing and widespread applications of the PEM NF membranes.

研究领域: 材料科学 · 环境工程 · 化学工程
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LANGMUIR · 2013 · IF 4.187

Ion Specificity at a Low Salt Concentration in Water–Methanol Mixtures Exemplified by a Growth of Polyelectrolyte Multilayer

Yunchao Long,Tao Wang,Lvdan Liu,Guangming Liu,Guangzhao Zhang

By use of a quartz crystal microbalance with dissipation (QCM-D), we have investigated the specific ion effect on the growth of poly(sodium 2-acrylamido-2-methylpropanesulfonate)/poly(diallyldimethylammonium chloride) multilayer at a salt concentration as low as 2.0 mM in water–methanol mixtures. QCM-D results demonstrate that specific ion effect can be observed in methanol and water–methanol mixtures though it is negligible in water. Moreover, the specific ion effect is amplified as the molar fraction of methanol (xM) increases from 0% to 75% but is weakened again with the further increase of xM from 75% to 100%. Nuclear magnetic resonance measurements reveal that the counterion–polyelectrolyte segment interactions may not account for the observed ion specificity. By extending the Collins’ concept of matching water affinities to methanol and water–methanol mixtures, we suggest that the ion–solvent interactions and the resulted counterion–charged group interactions are responsible for the occurrence of the specific ion effect. The conductivity measurements indicate that water and methanol molecules may form complexes, and the change of relative proportion of complexes with the xM causes the amplification or weakening of the specific ion effect.

CAS / MDL: 7398-69-8 27119-07-9
研究领域: 材料科学 · 物理化学
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JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION · 2023 ·Vol. 38 ·期 3 ·505-513 · IF 1.6

Au@Ag Core-shell Nanorods Self-assembled on Polyelectrolyte Multilayers for Ultra-High Sensitivity SERS Fiber Probes

Wang Wenbo,Xiong Wenhao,Long Yuting,Li Hong

We demonstrated a chemical process in the fabrication of a SERS fiber probe with an ultrahigh sensitivity. The synthesis was carried out by preparing Au@Ag core-shell nanorods (Au@Ag-NRs) self-assembled on polyelectrolyte (PE) multilayers, for which Au@Ag-NRs were controlled by adjusting the silver layer thickness. The effect of silver layer thickness of Au@Ag-NRs on the SERS performance of the fiber probe was investigated. The SERS fiber probe shows the best performance when the silver layer thickness is controlled at 8.57 nm. Under the condition of optimizing silver layer thickness, the fiber probe exhibits ultra-high sensitivity ( i e , 10 −10 M crystalline violet, CV), good reproducibility ( i e , RSD of 3.5%) and stability. Besides, electromagnetic field distribution of the SERS fiber probe was also investigated. The strongest enhancement is found within the core of fiber, whereas a weakened electromagnetic field exists in the fiber cladding layer. The SERS fiber probe can be a good candidate in ultra-trace detection for biomedical and environmental areas.

研究领域: 材料科学 · 生物医学工程 · 环境科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2020 · IF 3.573

Preparation of a Catalyst Layer by Layer-by-Layer Self-Assembly for Plate-Type Catalytic Membrane Microreactors

Ming Liu,Xun Zhu,Qiang Liao,Rong Chen,Dingding Ye,Gang Chen,Kun Wang,Sihong Song

Benefiting from the structures of membrane and microchannel, catalytic membrane microreactors are attractive for multiphase catalytic reactions. In addition to the membrane development, the fabrication of an efficient catalyst layer on a supporting layer is also significant for improving the performance of the membrane microreactor. In the present study, a plate-type catalytic membrane microreactor with the catalyst layer prepared by the layer-by-layer self-assembly technology along with the in situ adsorption and reduction was proposed. Herein, polydopamine (PDA) and polyelectrolyte multilayers (PEMs) were coated on the surface of the polydimethylsiloxane supporting membrane to adsorb more PdCl42– ions for the subsequent reduction. The synthesized catalyst layer termed as PDA/PEMs/Pd was characterized by analyzing the chemical composition and surface morphology. In addition, the catalytic performance of the developed microreactor was tested by using hydrogenation of nitrobenzene. The results showed that the use of both PDA and PEMs for preparing the catlayst layer yielded better conversion and durability than the use of PDA or PEMs alone. Besides, the nitrobenzene solution flow rate had an adverse impact of the nitrobenzene conversion resulting from the decreased residence time. With the increase of the hydrogen flow rate, the nitrobenzene conversion could be improved due to the increased gas permeation. The nirobenzene conversion also increased with a reduction in the initial concentration of nitrobenzene. In short, employing the layer-by-layer self-assembly technology for the catalyst layer preparation is promising for catalytic membrane microreactors toward multiphase catalytic reactions.

研究领域: 化学工程 · 材料科学
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ACS Applied Materials & Interfaces · 2017 · IF 7.504

Infusing Lubricant onto Erasable Microstructured Surfaces toward Guided Sliding of Liquid Droplets

Xia-chao Chen,Ke-feng Ren,Jing Wang,Wen-xi Lei,Jian Ji

Introducing a lubricant layer onto surfaces has emerged as a novel strategy to address a wide range of interface-related challenges. Recent studies of lubricant-infused surfaces have extended beyond repelling liquids to manipulating the mobility of fluids. In this study, we report a design of slippery surfaces based on infusing lubricant onto a polyelectrolyte multilayer film whose surface microstructures can be erased rapidly under mild condition. Unlike other lubricant-infused surfaces, the liquid movements (e.g., moving resistance and direction) on such surfaces can be manipulated via programming the surface microstructures beforehand. The work reported here offers a versatile design concept of lubricant-infused surfaces and may turn on new applications of this emerging class of bioinspired materials.

CAS / MDL: 78560-44-8
研究领域: 材料科学 · 表面工程 · 流体动力学 · 仿生材料
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JOURNAL OF CHROMATOGRAPHY A · 2017 · IF 3.981

Layer-by-layer self-assembly of polyelectrolyte multilayers on silica spheres as reversed-phase/hydrophilic interaction mixed-mode stationary phases for high performance liquid chromatography

Wenjie Zhao,Xiuming Jiang,Shujiao Ni,Yun Guo,Lijun He,Guoqiang Xiang,Shusheng Zhang

In this study, a series of stationary phases, comprising silica spheres and polyelectrolyte multilayers (PEMs) as the core and surface coating, respectively, were prepared via a layer-by-layer self-assembly approach for use in high-performance liquid chromatography. PEMs coatings were formed by the alternate deposition of positively charged poly(allylamine hydrochloride) and negatively charged poly(ethylene- alt -maleate) anions which were synthesized by esterification between poly(ethylene- alt -maleic anhydride) and n -alkyl alcohols (C n H 2n+1 OH, n   =   4, 8, 10, 12). The chromatographic performance and retention mechanism of the new stationary phases were evaluated in simultaneous reversed-phase/hydrophilic interaction mixed-mode chromatography using different solute probes, such as alkyl benzene, p -hydroxybenzoic acid and its esters, anilines, phenols, and pyrimidines. The separation performance of the new stationary phases was optimized by tuning the n -alkyl chain length of poly(ethylene- alt -maleate) and bilayer numbers of PEMs. These results indicated that the new stationary phases demonstrate promise for the simultaneous separation of complex hydrophobic and hydrophilic samples with high selectivity.

研究领域: 分析化学 · 材料科学
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BIO-MEDICAL MATERIALS AND ENGINEERING · 2014 · IF 0.847

pH-responsive mesoporous silica nanocarriers based on layer-by-layer self-assembly

Hong-Yu Zhang,Yan-Fang Sun,Yu-Long Sun,Ming Zhou

Significant progress has been achieved in the field of pH-sensitive drug delivery system in recent years. For layer-by-layer self-assembly nanocarriers, various pH values can induce the change of permeability and structural stability of the outer polyelectrolyte multi-layers, resulting in the release of the loaded drug. In the present study, carboxyl-modified mesoporous silica nanoparticles (MSNs-COOH) were prepared as reservoirs to hold model cargo, i.e. Rhodamine B (RhB). Polycations, including 1, 4-butanediamine (BDA)-modified linear poly (glycerol methacrylate) (L-B) or BDA-modified star-shaped poly (glycerol methacrylate) (S5-B) and 1,2-ethanediamine (EDA)-modified star-shaped poly (glycerol methacrylate) (S5-E), and polyanion, i.e. poly (acrylic acid) (PAA), are self-assembled by electrostatic interactions as coating. The loading process of RhB was characterized by transmission electron microscopy, Fourier transform infrared spectroscopy, thermo-gravimetric analysis, and dynamic light scattering, and the release of RhB was controlled by changing the pH of phosphate buffer saline. The results showed that the loading capacity and entrapment efficiency of RhB were the highest for S5-B/PAA, which were 10.1% and 44.4%, respectively. In addition, the release of RhB was about 90% at pH 2.0 and 35% at pH 7.4, which was indicative of obvious pH-responsivity. The MSNs-COOH coated by S5-B/PAA proposed in the present study show potential applications in targeted drug delivery.

研究领域: 纳米技术 · 材料科学 · 药剂学 · 生物医学工程 · 化学工程
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ACS Applied Materials & Interfaces · 2016 · IF 7.145

Improved Endothelial Function of Endothelial Cell Monolayer on the Soft Polyelectrolyte Multilayer Film with Matrix-Bound Vascular Endothelial Growth Factor

Hao Chang,Mi Hu,He Zhang,Ke-feng Ren,Bo-chao Li,Huan Li,Li-mei Wang,Wen-xi Lei,Jian Ji

Endothelialization on the vascular implants is of great importance for prevention of undesired postimplantation symptoms. However, endothelial dysfunction of regenerated endothelial cell (EC) monolayer has been frequently observed, leading to severe complications, such as neointimal hyperplasia, late thrombosis, and neoatherosclerosis. It has significantly impeded long-term success of the therapy. So far, very little attention has been paid on endothelial function of EC monolayer. Bioinspired by the microenvironment of the endothelium in a blood vessel, this study described a soft polyelectrolyte multilayer film (PEM) through layer-by-layer assembly of poly(l-lysine) (PLL) and hyaluronan (HA). The (PLL/HA) PEM was chemically cross-linked and further incorporated with vascular endothelial growth factor. It demonstrated that this approach could promote EC adhesion and proliferation, further inducing formation of EC monolayer. Further, improved endothelial function of the EC monolayer was achieved as shown with the tighter integrity, higher production of nitric oxide, and expression level of endothelial function related genes, compared to EC monolayers on traditional substrates with high stiffness (e.g., glass, tissue culture polystyrene, and stainless steel). Our findings highlighted the influence of substrate stiffness on endothelial function of EC monolayer, giving a new strategy in the surface design of vascular implants.

CAS / MDL: 25952-53-8 106627-54-7
研究领域: 生物材料 · 组织工程 · 生物医学工程 · 细胞生物学
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JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION · 2024 ·Vol. 39 ·期 1 ·7-16 · IF 1.3

Controllable Synthesis of Au NRs and Its Flexible SERS Optical Fiber Probe with High Sensitivity

Xiong Wenhao,Wang Wenbo,Long Yuting,Li Hong

The surface-enhanced Raman scattering (SERS) optical fiber probes were successfully prepared by self-assembling on polyelectrolyte multilayers. Gold nanorods (Au NRs) were used as SERS enhancement material to give excellent biological affinity and stability to the SERS optical fiber probes. Au NRs were synthesized by seed growth method. The synergistic effect between AgNO 3 and surfactant was investigated, and the highest yield was found when AgNO 3 was 500 uL. Meanwhile, different SERS optical fiber probes were obtained by selecting silane coupling agent, polyelectrolyte multilayer and graphene oxide (GO) to treat quartz fiber. It was found that the SERS optical fiber probes obtained by the self-assembled on polyelectrolyte multilayers method performed better than those by other methods. In addition, Mapping was combined with finite element simulation to analyze the electromagnetic field distribution at the fiber end face. The electromagnetic field distribution of Au NRs was investigated, the difference of electromagnetic field intensity around the Au NRs with different arrangements was compared, the strongest signal was obtained when the Au NRs were head-to-head. Finally, sensitivity of the optimized SERS optical fiber probes could reach 10 −9 mol/L, with excellent stability and repeatability.

研究领域: 纳米技术 · 分析化学 · 光学 · 材料科学 · 生物物理学
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RSC Advances · 2021 ·Vol. 11 ·期 42 ·26160-26167 · IF 3.361

“Kill-release” antibacterial polysaccharides multilayer coating based therapeutic contact lens for effective bacterial keratitis treatment

Rui Wang,Duoduo Lu,Hui Wang,Haoyu Zou,Ting Bai,Chulei Feng,Quankui Lin

Contact lenses (CLs) are an important medical device for ophthalmic disease treatment. They can be used not only to correct refractive errors, such as myopia, but also can serve as a drug carrier for ocular surface disease treatment. In this study, a therapeutic CL was designed for bacterial keratitis treatment by constructing an antibacterial surface coating via a layer-by-layer (LbL) electrostatic self-assembly method. Vancomycin-incorporated chitosan nanoparticles were firstly prepared by ionic condensation of sodium tripolyphosphate (abbreviated as CTVNP). The positively charged CTVNP were then used for LbL deposition with negatively charged heparin (HEP), obtaining a (HEP/CTVNP)n polyelectrolyte multilayer on the CL surface. It is shown that such antibiotic incorporated surface coating doesn't influence the light transmittance of the CL, so it should not affect the patients' visual acuity when wearing them. The in vitro bacteriostatic effect evaluation was performed via live and dead bacteria staining and scanning electron microscope (SEM), which demonstrated the effective antibacterial property of such a surface. The fabricated therapeutic CL was then used to treat bacterial keratitis on a rabbit model. The results showed that such CL could effectively control the development of the bacteria-infected cornea and had a significant therapeutic effect.

CAS / MDL: 75-47-8 603-35-0
研究领域: 眼科学 · 材料科学 · 药学 · 生物医学工程
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Journal of Biophotonics · 2023 · IF 2.8

Trace detection of canine distemper virus based on Michelson-interferometer sensing probe

Xinyu Zhang,Xiangyu Hou,Wenlin Feng

A single-mode-fiber (SMF)-multimode-fiber (MMF)-tri-core-fiber (TCF) Michelson probe structure is proposed for trace detection of canine distemper virus (CDV). One end of the TCF is cut flat and fused with the multimode fiber, and the other end is coated with a silver film to enhance the reflection, and an optic-fiber sensing probe with SMF-MMF-TCF structure is obtained. The (PDDA/PSS) 3 multilayer film is modified on the surface of the fiber by layer-by-layer self-assembly method as a polyelectrolyte binder to immobilize CDV antibodies to form a (PDDA/PSS) 3 /CDV antibody composite membrane for specific detection of CDV antigens. The response-recovery test of the sensor is performed to verify its repeatability. The detection limit, the sensitivity, and the linear fitting degree for CDV antigen are 0.1236 pg/mL, 1.1776 dB/(pg/mL), and 0.9899, respectively. At the same time, the stability, selectivity, and clinical samples of the sensors were also verified.

CAS / MDL: 50-99-7 1310-58-3
研究领域: 光学传感 · 生物传感器 · 兽医学 · 纳米技术
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2016 · IF 3.902

Stiffness of polyelectrolyte multilayer film influences endothelial function of endothelial cell monolayer

Hao Chang,He Zhang,Mi Hu,Jia-yan Chen,Bo-chao Li,Ke-feng Ren,M.Cristina L. Martins,Mário A. Barbosa,Jian Ji

Endothelialization has proved to be critical for maintaining long-term success of implantable vascular devices. The formation of monolayer of endothelial cells (ECs) on the implant surfaces is one of the most important factors for the endothelialization. However, endothelial function of regenerated EC monolayer, which plays a much more important role in preventing the complications of post-implantation, has not received enough attention. Here, a vascular endothelial growth factor (VEGF)-incorporated poly( l -lysine)/hyaluronan (PLL/HA) polyelectrolyte multilayer film was fabricated. Through varying the crosslinking degree, stiffness of the film was manipulated, offering either soft or stiff film. We demonstrated that ECs were able to adhere and proliferate on both soft and stiff films, subsequently forming an integrated EC monolayer. Furthermore, endothelial functions were evaluated by characterizing EC monolayer integrity, expression of genes correlated with the endothelial functions, and nitric oxide production. It demonstrated that EC monolayer on the soft film displayed higher endothelial function compared to that on the stiff film. Our study highlights the influence of substrate stiffness on endothelial function, which offers a new criterion for surface design of vascular implants.

CAS / MDL: 25952-53-8 106627-54-7
研究领域: 生物材料 · 组织工程 · 生物医学工程
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