MICROCHIMICA ACTA
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2025
·Vol. 192
·期 5
·1-9
·
IF 5.3
Zhang Guiyun,Lai Zhiwei,Xie Jianhua,Yang Weiqiang
Methylmercury (CH 3 Hg + ), a lipophilic environmental pollutant, accumulates in fish, shellfish, and other organisms, posing significant risks to human health through the food chain. Developing a convenient and sensitive analytical method for CH 3 Hg + detection is crucial for reducing costs and enhancing the efficiency of food safety testing. In this study, we prepared an octyl-modified silica isoporous membrane on the indium tin oxide (ITO) electrode (Octyl-SIM/ITO) via the electrochemical-assisted self-assembly (EASA) method using octyltrimethoxysilane (O-TES) as the functional organosilane. The Octyl-SIM/ITO electrode exhibits vertically-ordered nanochannels and strong hydrophobic affinity, enabling selective penetration and enrichment of weakly polar analytes. Utilizing square wave anodic stripping voltammetry (SWASV), the Octyl-SIM/ITO electrode demonstrates superior electrochemical response signals for CH 3 Hg + detection, achieving a detection limit as low as 4 nM. This method allows for accurate and reproducible detection of CH 3 Hg + in fish and oyster samples with minimal sample preparation, offering promising potential for portable in situ detection. Graphical
研究领域:
环境科学
·
分析化学
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2019
·
IF 7.015
Juan Cheng,Miao Xu,Panpan Cheng,Wanna Zhang,Nan Li,Yong Wang,Jingying Yang,Kaiyuan Liang,Peng Li,Haizhou Yu,Xiaoyan Qiu
As a representative amphiphilic block copolymer , polystyrene- block -poly (acrylic acid) (PS- b -PAA) has great potential in biomedical applications owing to its pH-responsiveness, antibacterial property and biocompatibility. Self-assembly of PS- b -PAA has been widely investigated with regard to micelles and thin films . Whereas, it is difficult to precipitate PS- b -PAA in water to make membrane due to the high hydrophilicity of PAA blocks. Herein, a process is described to fabricate PS- b -PAA isoporous membranes by combining self-assembly of metal-block copolymer complexes and non-solvent induced phase separation. Different antibacterial metal ions were doped in PS- b -PAA casting solution, which not only enhanced the mechanical property significantly, but also adjusted the pore size of the membranes. The membranes exhibited a pH-responsive release property and excellent separation performance based on size or charge differences. Moreover, the antifouling property was significantly enhanced through the synergistic effect of antibacterial metal ions and PAA segments.
研究领域:
材料科学
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生物医学工程
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DOI
高影响因子
ACS Sensors
·
2017
·
IF 0
Lisiqi Xie,Xiao Huang,Bin Su
A portable amperometric ion sensor was fabricated by integrating silica isoporous membrane (SIM) and organogel composed of polyvinyl chloride and 1,2-dichloroethane (PVC-DCE) on a 3D-printed polymer chip. The detection of ionic species in aqueous samples could be accomplished by adding a microliter of sample droplet to the sensor and by identifying the ion-transfer potential and current magnitude at the water/organogel interface array templated by SIM. Thanks to the ultrasmall channel size (2–3 nm in diameter), high channel density (4 × 108 μm–2), and ultrathin thickness (80 nm) of SIM, the ensemble of nanoscopic water/organogel (nano-W/Gel) interface array behaved like a microinterface with two back-to-back hemispherical mass diffusion zones. So, the heterogeneous ion-transfer across the nano-W/Gel interface array generated a steady-state sigmoidal current wave. The detection of choline (Ch) and its derivatives, including acetylcholine (ACh), benzoylcholine (BCh), and atropine (AP), in aqueous samples was examined with this portable sensor. Using differential pulse stripping voltammetry (DPSV), the quantification of these analytes was achieved with a limit of detection (LOD) down to 1 μM. Moreover, the portable ion sensor was insensitive to various potential interferents that might coexist in vivo, owing to size-/charge-based selectivity and antifouling capacity of SIM. With this priority, the portable ion sensor was able to quantitatively determine Ch and its derivatives in diluted urine and blood samples. The LODs for Ch, ACh, AP, and BCh in urine were 1.12, 1.30, 1.08, and 0.99 μM, and those for blood samples were 3.61, 3.38, 2.32, and 1.81 μM, respectively.
研究领域:
分析化学
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生物医学工程
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DOI
PubMed
TALANTA
·
2024
·
IF 5.6
Qingda Yao,Qiaoling Fang,Zhiping Song,Jiancong Ni,Weiqiang Yang,Zhenyu Lin
Acid vapors emitted by chemical industries pose an increasing threat to public health. The development of a cost-effective sensor for the on-site and real-time monitoring of environmental acid vapor is of great significance. Aggregation-induced emission (AIE) luminogens overcome the aggregation-caused quenching effect and exhibit intense fluorescence when supported in the solid matrices. Silica isoporous membrane (SIM), characterized by vertically ordered nanochannels, holds great promise as a platform for encapsulating AIE luminogens and enabling gas sensing applications. The SIM containing surfactant micelles was prepared on an ITO electrode to obtain the M-SIM/ITO, and Tetrakis(4-carboxyphenyl)ethylene (TCPE) was employed as the investigated AIE luminogen. Upon application of positive potential, the negatively charged TCPE molecules were driven into the vertically ordered nanochannels, resulting in observable AIE fluorescence. By investigating the electrophoresis conditions such as TCPE charge, nanochannel microenvironment, and driving electric field, the AIE mechanism within the nanochannels was elucidated. The fluorescence of TCPE@M-SIM/ITO exhibited high sensitivity towards acid vapor and displayed reversible changes during the absorption and desorption processes. This behavior can be attributed to the SIM's strong absorption capability towards acid vapor as well as the reversible conversion of acid vapor on TCPE aggregates. This work presented an innovative methodology for studying luminophores within an orderly nanoconfined space, leading to a new perspective on the AIE mechanism.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2016
·
IF 2.822
Lisiqi Xie,Xiao Huang,Xingyu Lin,Bin Su
Miniaturization of the interface between two immiscible electrolyte solutions (ITIES) brings the benefits of enhanced mass transport in comparison with the macroscopic ITIES, similar to those observed with an ultramicroelectrode. In this work, ultrathin free-standing silica isoporous membrane (SIM, 80 nm in thickness) consisting of a high density of perforative channels with a uniform size (2–3 nm in diameter) was used to construct nanoscopic ITIES (nano-ITIES) arrays. Electrochemical characterization of the nano-ITIES array by studying the ion-transfer voltammetric behavior of tetra- n -propylammonium (TPrA + ) suggested the domination of hemispherical molecular diffusion. The effect of trans-membrane resistance on the heterogeneous ion transfer was investigated by varying the supporting electrolyte concentration in both phases, which was found to be negligible due to the ultrathin thickness and high channel density of SIM. In addition, the nano-ITIES array exhibited excellent charge selectivity towards ionizable species due to the overlap of electrical double layer in the ultrasmall silica channels, which could be modulated by the supporting electrolyte concentration, aqueous solution pH and channel surface modification. These findings provide the basis for the nano-ITIES array to be used in ion detection and separation.
研究领域:
材料科学
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电化学
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纳米技术
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2018
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IF 6.578
Wanhao Wu,Qian Yang,Bin Su
Nanoporous molecular sieving membranes with high densities of uniform pores over macroscopic areas are highly desired to achieve a high permeation rate and a high molecular selectivity. In the first part of this work, our primary calculation using a quasi-steady state model indicates that the effective way of achieving a high molecular permeation is to increase the pore density and area of sieving membrane. Then the experimental work has been projected to prepare the centimeter-scale continuous silica isoporous membrane (SIM) consisting of parallel nanochannels under the support of porous polyethylene terephthalate (PET) film. Without using any expensive facilities or harsh conditions, simple wet-chemistry growth followed by membrane transfer was used to produce SIM with a large area up to 2.5 cm × 2.5 cm with ultrasmall thickness (ca. 90 nm) and high pore density (ca. 4.0 × 10 12 cm −2 ). The prepared SIM-PET membrane demonstrated a molecular permeation rate almost one order of magnitude larger than commercial dialysis and nanoporous polycarbonate membranes. Moreover, thanks to uniform pore size (2.3 nm in diameter) and negatively charged surface of silica nanochannels, the membrane showed a precise selectivity at the molecular level in terms of molecular size and charge. Simultaneous achievement of high permeability and high selectivity, as well as simple fabrication and low cost, proves the potential of centimeter-scale SIM in molecular sieving and other applications.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Wenjing Wang,Zixiong Wang,Xiaomin Sun,Zhuan Yi,Congjie Gao
Isoporous block copolymer membranes with high porosity and narrow pore size distribution have been viewed as ideal membrane platforms for precise separation of similarly sized particles or solutes. However, tailored made fabrication of solvent-resistant isoporous membranes with switchable pores and rigid pores for customizable sieving have been rarely reported. Herein, we show that site-selective hyper-crosslinking is effective and robust to prepare such membranes from polystyrene- block -poly(4-vinylpyridine) (PS- b -P4VP). The selective crosslinking in PS domains endows the membrane with excellent solvent resistance and structural stability. Since not participated in the crosslinking reaction, the P4VP brushes located in pore walls endow the crosslinked membranes with adaptive pore size, switchable permeance and tunable rejections that vary with Hansen solubility parameter of solvents. Moreover, by a facile while complete etching the P4VP from pores, the switchable performance is removed and resultant membranes show rigid pore characteristics and constant rejections. Crosslinked membranes with either switchable pores or rigid-likes pores exhibit superior long-term stability (30 days) in harsh solvents. This work presents a top-down method to construct highly stable isoporous membranes with both switchable and rigid pore characteristics from the same block copolymer , which will shed the light on precisely tailoring the pore size and pore rigidity for crosslinked isoporous membranes that will not only enable the tailored sieving but also the modelling of solvent flowing behaviours in nanopores .
研究领域:
材料科学
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分离技术
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DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 5
·2385-2391
·
IF 10.733
Fei Yan,Lina Yao,Kenxin Chen,Qian Yang,Bin Su
Artificial solid-state nanochannels are capable of regulating unipolar ion transport in their confined space and thus converting the Gibbs free energy stored in the salinity gradients to electricity. In order to achieve a large conversion efficiency, highly ion-selective and permeable nanochannel membranes are inevitably desired. In this work we report the salinity energy conversion using an ultrathin silica isoporous membrane (SIM, ∼90 nm in thickness) that consists of straight, uniform and close packed nanochannels (diameter, 2–3 nm; pore density, ∼4 × 1012 cm−2, corresponding to a porosity of 16.7%). Thanks to its unique structure and negatively charged surface, the SIM displayed excellent cation selectivity and meanwhile preserved a high ionic flux, and was capable of harnessing the osmotic energy efficiently upon mixing artificial seawater and river water. We rationalized the ion distribution inside the nanochannels in the presence of salinity gradients and the effect of the channel length on the energy conversion efficiency by finite element simulations. The simulated results suggest that short nanochannels with an ultrasmall dimeter of ∼2.3 nm and a length of ∼100 nm possess excellent cation selectivity. Both experimental and theoretical results suggest that the SIM is a highly potential material in salinity energy conversion.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2023
·
IF 4.5
Haiming Lv,Guiyun Zhang,Weiqiang Yang,Xiaohui Dai,Yang Huang,Jiancong Ni,Qingxiang Wang
Heavy metal ions (HMIs) pollutant is a serious environmental problem and the on-site supervision exhibits increasing urgency. Silica isoporous membrane (SIM) has the characteristic of anti-fouling while screen-printed carbon electrode (SPCE) is a universal detection platform that is feasible to commercialize. According to the principle of electrochemically assisted self-assembly (EASA), SIM was prepared on the SPCE surface for the first time. A highly ordered mesoporous silica membrane was obtained when a cathodic current was applied to the electro-activated SPCE. The developed SIM/SPCE was used for detecting the soil Cd 2+ , Pb 2+ , Cu 2+ , and Hg 2+ by the square wave anodic stripping voltammetry (SWASV). Owing to the large specific surface area of SIM, the SIM/SPCE responded HMIs with enhanced SWASV signals. The detection limits of Cd 2+ , Pb 2+ , Cu 2+ , and Hg 2+ were 9.3, 1.1, 16.2, and 1.4 nM, respectively. More importantly, the SIM/SPCE had a fine anti-fouling capability arising from steric exclusion and selective permeation. The soil samples were only diluted with buffer and the analytical performance was not decreased, suggesting a free of tedious sample pretreatments. Additionally, the universal use of SPCE endows the SIM/SPCE with more compatibility for instrumentation, thus driving an attractive application in the field of portable detection.
研究领域:
环境科学
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分析化学
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材料科学
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电化学
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产品关联
DOI
高影响因子
MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 10
·1-9
·
IF 5.3
Yang Weiqiang,Fang Qiaoling,Lv Haiming,Zhang Guiyun,Ni Jiancong,Lin Zhenyu
A phenyl-modified silica isoporous membrane (Ph-SIM) was prepared on the indium-tin-oxide (ITO) electrode using the electrochemically assisted self-assembly (EASA) method. The resulting Ph-SIM preserved vertically ordered nanochannels while exhibiting outstanding hydrophobicity due to the incorporation of phenyl groups within the nanochannels. As a result, the Ph-SIM/ITO sensor exhibited a remarkable affinity for PCNB extraction through hydrophobic interactions, leading to high detection sensitivity. The electrochemical response showed a linear enhancement with the logarithmic concentration of PCNB ranging from 0.1 to 20.0 µM, and the limit of detection was 4.64 nM. Practical results demonstrated that the Ph-SIM/ITO sensor possessed good anti-fouling capability and robust stability, making it a promising candidate for portable detection of non-polar contaminants. Graphical Abstract
研究领域:
材料科学
·
分析化学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子