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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Electrochemiluminescence-Based Single-Particle Tracking of the Biomolecules Moving along Intercellular Membrane Nanotubes between Live Cells

Zhi-Gang Wang,Yusi Hu,Hao-Yang Liu,Hai-Yan Wen,Bao-Ping Qi,Shu-Lin Liu

Electrochemiluminescence (ECL) imaging, a rapidly evolving technology, has attracted significant attention in the field of cellular imaging. However, its primary limitation lies in its inability to analyze the motion behaviors of individual particles in live cellular environments. In this study, we leveraged the exceptional ECL properties of quantum dots (QDs) and the excellent electrochemical properties of carbon dots (CDs) to develop a high-brightness ECL nanoprobe (CDs-QDs) for real-time ECL imaging between living cells. This nanoprobe has excellent signal-to-noise ratio imaging capabilities for the single-particle tracking (SPT) of biomolecules. Our finding elucidated the enhanced ECL mechanism of CDs-QDs in the presence of reactive oxygen species through photoluminescence, electrochemistry, and ECL techniques. We further tracked the movement of single particles on membrane nanotubes between live cells and confirmed that the ECL-based SPT technique using CD-QD nanoparticles is an effective approach for monitoring the transport behaviors of biomolecules on membrane nanotubes between live cells. This opens a promising avenue for the advancement of ECL-based single-particle detection and the dynamic quantitative imaging of biomolecules.

研究领域: 细胞生物学 · 分析化学
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AICHE JOURNAL · 2025 · IF 4

Manipulating central intermolecular interaction in confined nanochannels for fast transport

Jingjing Chen,Yongjian Yang,Tao Zhou,Xiaoli Wu,Chongchong Chen,Ye Wan,Jianhua Liu,Zhirong Yang,Jingtao Wang

The study of molecule transport within confined nanochannels is crucial to developing high-performance membranes. Previous studies mainly focus on the interfacial molecule transport; however, the central molecule transport, equally crucial, has been disregarded. Herein, vertically aligned vermiculite-based (Vr-based) membranes with long-range nanochannels are engineered to ensure a stable flow. Meanwhile, the channel surfaces are functionalized (–CH 3 , –NH 2 , and –CF 3 groups) to tune the interaction with interfacial molecules, thus affecting the intermolecular interaction of central molecules. We demonstrate that strong channel-molecule interaction between polar walls and protonic solvents can impede the formation of hydrogen-bond networks in central molecules, thus reducing the central intermolecular interaction and enabling fast transport. For instance, the Vr-CF 3 membrane displays a 69% improvement in water permeance in comparison to the Vr-CH 3 membrane, achieving 13.0 LMH bar −1 . Nevertheless, nonpolar walls with weak channel-molecule interaction show uninfluenced intermolecular interaction, giving comparable transport ability for both protonic and non-protonic solvents.

研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Precise identification and transport of specific molecules through framework-functionalized membranes with multiple binding sites

Kaicheng Zhang,Yue Li,Zequan Diao,Hang Cui,Faguang Ma,Ming Yan,Yilin Wu

Membranes with specific-recognition and superfast-filtration have significant practical applications in water purification and chiral separation. However, membrane technique still remains challenging to high selectivity and permeation in aqueous-and-organic solvents. Here, we reported a new approach to designing framework-functionalized membranes with multiple binding sites (FMMBSs) that enabled structure&size-exclusion selectivity and fast transport performance towards specific compound of shikimic acid (SA). The as-prepared FMMBSs, based on intrinsic core-shell structure of the boronate-affinity sol-gel imprinted polymers, demonstrated that exquisite control over polymerization pattern and functionalization of characteristic membrane construction played important roles in achieving fast molecule transport combined with high molecular selectivity. The superior property of the membrane-based core-shell structure had been initially demonstrated by testing nitrogen adsorption capacity, showing about a 3.0 times higher result (63.65 cm 3 /g) than that of original membrane (20.71 cm 3 /g). These framework-functionalized membranes were then regarded as the platforms to construct the FMMBSs through a first-time-developed boronate-affinity sol-gel imprinting strategy. Therefore, the FMMBSs always kept remarkably static rebinding capacity (45.48 mg g −1 ) and perm-selectivity factors (>10). The dynamic transport results showed that much higher SA-based rebinding capacities than that of other molecules could be still observed under pump-pressure-driven for a long time, which strongly confirmed the preparation of high-efficiency selective membrane separation system. The strategy of introducing framework-functionalized structure on porous membrane would offer a window of opportunity for preparation of high-intensitive selective separation membrane systems not only for continuous high permeability, but also for competitive selectivity.

研究领域: 材料科学 · 环境科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Conically channeled membranes designed for fast and efficient transport of macromolecules

Lu Tao,Xu Yang,Qi Liu,Xingchi Liu,Xinru Bao,Yumeng Li,Jiawei Yin,Yinhua Wan,Guoqiang Chen

Transport channels for the separation and sensing of biomacromolecules, especially therapeutic biodrugs, have attracted substantial interest. The growing attention underscores the critical need for appropriate control strategies over membrane channels characteristics including size, structure and shape. While homoporous membranes featuring conical nanopores have demonstrated excellent performance in facilitating the transport of small molecules and ions, the potential advantages of membranes with conical micropores for biomacromolecule transport remain inadequately explored. This gap primarily arises from the difficulty in scaling the cone tip to the micrometer range using traditional etching techniques. To address this challenge, we developed a shape-and-size sequential etching method with enhanced controllability, enabling the fabrication of microscale conical channels. A theoretical model of the etching period was proposed for etching scheme determination. Key experimental factors, including etching time, temperature, and adding ethanol as an additive, were investigated and shown to significantly influence etching performance. Notably, the as-prepared membrane with conical channels led to significantly increased fluxes (8.10 vs 3.84 μL/h at 0.08 MPa) and enhanced dynamic binding capacity (476.03 vs 382.88 pmol/cm 2 ), exhibiting remarkable advantages over the cylindrical-channel membrane. Overall, this sequential etching method allows customizable membrane fabrication with precise conical microchannels, offering a versatile membrane-based platform for a broad spectrum of challenging biopharmaceutical separation, biosensing, and drug delivery.

研究领域: 生物工程 · 制药工程 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Precise identification and ultrafast transport of specific molecules with nanofluid-functionalized imprinted membrane

Kaicheng Zhang,Ming Yan,Yue Li,Faguang Ma,Yilin Wu

Membrane-based imprinted sites for achieving specific molecule transport and precise recognition have great potential to revolutionize nanofiltration technology . Nonetheless, how to efficiently prepare imprinted membrane structures with accurate identification - ultrafast molecular transport - high stability in mobile phase remains a key issue and serious challenge. Herein, we have developed a dual-activation strategy to constructing nanofluid-functionalized membranes with double imprinted nanoscale channels (NMDINCs), realizing ultrafast transport performance as well as structure&size-exclusion selectivity in allusion to particular compounds. The resultant NMDINCs, founded on principal nanofluid-functionalized construction companied by the boronate affinity sol-gel imprinting systems, illustrated that delicate regulation towards polymerization framework as well as functionalization belonging to distinctive membrane structures was crucial for realizing ultrafast molecules transport combined with prominent molecules selectivity. The synergistic recognition of covalent bonds and non-covalent bonds driven by two functional monomers effectively realized the selective recognition to template molecules, leading to the high selective separation factors of Shikimic acid (SA)/ Para hydroxybenzoic acid(PHA), SA/ P nitrophenol(PN)and catechol(CL)for 8.9, 8.14 and 7.23, respectively. The dynamic consecutive transport outcomes exhibited that numerous SA-dependent recognition sites could still keep reactivity under pump-driven permeation pressure for appreciable time, forcefully proving the successful construction as to high-efficiency membrane-based selective separation system. It is anticipated that this strategy as to the in situ introduction of nanofluid-functionalized construction into porous membrane would hold great promise in preparing high-intensities membrane-founded discriminating separation systems, which was equipped with prominent consecutive permeability as well as excellent selectivity.

研究领域: 材料科学 · 化学工程 · 纳米技术 · 分离技术
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ANALYTICAL CHEMISTRY · 2023 · IF 7.4

Quantitative Ratiometric Biosensors Based on Fluorescent Ferrocene-Modified Histidine Dipeptide Nanoassemblies

Jia Kong,Shixuan Zhao,Xue Han,Wenxin Li,Jiaxing Zhang,Yuefei Wang,Xihui Shen,Yinqiang Xia,Zhonghong Li

Fluorescent proteins (FPs) provide a ratiometric readout for quantitative assessment of the destination of internalized biomolecules. FP-inspired peptide nanostructures that can compete with FPs in their capacity are the most preferred building blocks for the synthesis of fluorescent soft matter. However, realizing a ratiometric emission from a single peptide fluorophore remains exclusive since multicolor emission is a rare property in peptide nanostructures. Here, we describe a bioinspired peptidyl platform for ratiometric intracellular quantitation by employing a single ferrocene-modified histidine dipeptide. The intensiometric ratio of green to blue fluorescence correlates linearly with the concentration of the peptide by three orders of magnitude. The ratiometric fluorescence of the peptide is an assembly-induced emission originating from hydrogen bonds and aromatic interactions. Additionally, modular design enables ferrocene-modified histidine dipeptides to use as a general platform for the construction of intricate peptides that retain the ratiometric fluorescent properties. The ratiometric peptide technique promises flexibility in the design of a wide spectrum of stoichiometric biosensors for quantitatively understanding the trafficking and subcellular fate of biomolecules.

研究领域: 生物化学 · 纳米技术 · 分子生物学 · 生物物理学 · 分析化学
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