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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Directional and on-demand ion transport regulated by pH and voltage in submicrochannel heteromembrane based on conducting polymer

Yuan-Ju Tang,Shu-Jie Zhang,Zi-Tao Zhong,Bin Zhang,Wen-Ming Su,Guo-Ping Wang,Yuan-Di Zhao

The construction of porous ion channels with ion current rectification (ICR) at the submicron scale has great significance for the development of large-area bionic ion channel devices. In this manuscript, one kind of heterogeneous membrane with asymmetric composition, geometry and wettability was prepared by simple drop-coating of the neutral hydrophobic conducting polymer precursor and in-situ thermal polymerization on cylindrical submicron scale anodic aluminum oxide channels (D≈269 nm) at 150 °C. ICR in the submicrochannel heterogeneous membrane was successfully achieved due to the asymmetric charge distribution induced by asymmetric pH gradient. Furthermore, the rectification ratio ( R ic : 1.6 ∼ 42.8) could be effectively regulated by multiple drop-coating, the electrolyte concentration (0.01 mM ∼ 1 M) and pH gradient (3 ∼ 11). Finally, through the permeation experiment of anionic dye and cationic dye, the mechanism of the synergistic effect of surface charge and electrophoresis on the ion selectivity and ICR was discussed, and it was successfully applied to the directional and on-demand transport of anionic and cationic ions under the regulation of pH gradient and voltage driving. It has important potential applications in the treatment of pollutants, the purification of water and energy conversion etc.

研究领域: 生物物理学 · 材料科学 · 仿生学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Constructing oxidized carbon spheres-based heterogeneous membrane with high surface energy for energy-free water purification

Jincui Gu,Tianyu Chen,Peng Xiao,Feng Ni,Luke Yan,Yujing Nie,Tao Chen

Producing affordable freshwater becomes increasingly essential. Membrane separation technology offers an unprecedented opportunity, but they typically use fuel energy during the separation process. Therefore, it is a severe challenge to construct an advanced membrane for energy-free water purification. Herein, for the first time, we reported a heterogeneous membrane for pressure-free water purification. Oxidized carbon spheres (OCS) membrane was optimized by the coordinated modification of polydopamine (PDA) and tetrakis(hydroxymethyl)phosphonium chloride (THPC). Remarkably, the OCS@PDA membrane was progressively hydroxylated due to the THPC’s superb water-binding ability. Therefore, the OCS@PDA/THPC membrane demonstrated higher surface free energy and better hydrophilic capacity than the other membranes. Under the combined effect of abundant porous geometry and strong charge interaction, this membrane presented a splendid screening performance for various dye molecules without extra pressure. In addition, its separation throughput can be improved by regulating the external temperature. This work may offer a straightforward manner to handle the relationship between membrane structure and performance for pressure-free water purification.

研究领域: 材料科学 · 环境工程
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

pH and non-enzymatic glucose response at ultra-low concentration using submicrochannel heterogeneous membrane

Yuan-Ju Tang,Kai Cheng,Lin-Fang Tan,Xiao-Ting Xie,Bin Zhang,Wen-Ming Su,Yuan-Di Zhao,Qiu-Ran Xu

The construction of solid nanochannel-based biosensor with submicron pore size has great significance to the analysis of biomolecule with high sensitivity and low detection limit. In this paper, a submicrochannel heterogeneous membrane with asymmetric geometry is prepared as the base by combining thermo-crosslinked hydrophobic conducting polymer and porous anodic aluminium oxide channel (AAO) with submicron pore size (269 nm). After the polydopamine-Au multilayer assembly, a large number of Au nanoparticles with adjustable size (∼10 and 89 nm) and density are in situ generated and fixed on the inner wall of AAO. Then 4-mercapto phenylboric acid with high density is grafted through Au-S bond to construct the submicrochannel heterogeneous membrane with the characteristic of ion current rectification in response to pH and saccharide. Benefit from the blocking effect of hydrophobic conducting polymer and the multilayer assembly of polydopamine-Au, the current of background response by the membrane device is effectively reduced, the ion current rectification strength can be effectively regulated in the range of pH 3–9, and the response to ultra-low glucose concentration without enzyme is achieved in the linear range of 1 pM-0.1 μM. A universal substrate platform is provided for the construction of solid nanochannel-based biosensor with submicron pore size.

CAS / MDL: 62-31-7 626-23-3 77-86-1
研究领域: 生物传感 · 材料科学 · 分析化学
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ANALYST · 2021 ·Vol. 146 ·期 22 ·6815-6821 · IF 4.616

Controllable ion transport induced by pH gradient in a thermally crosslinked submicrochannel heterogeneous membrane

Yuan-Ju Tang,Shu-jie Zhang,Zi-Tao Zhong,Wen-Ming Su,Yuan-Di Zhao

Solid-state nanochannels have attracted considerable attention for their similar ion transport properties to biological ion channels. The construction of porous ion channels with good stability at the submicro/micrometer scale is very beneficial to develop large-area ion channel devices. In this manuscript, based on in-situ thermal crosslinking of a small organic molecule containing triphenylamine and styrene groups, we construct a heterogeneous membrane with asymmetrical charge and wettability on cylindrical anodic aluminum oxide (AAO) channels (D ≈ 319 nm). This heterogeneous membrane has typical ion current rectification characteristics with a high rectification ratio of 36.9 and good stability. This work provides an effective strategy for the construction of submicrochannel heterogeneous membranes and also broadens the application range of bionic ion channels.

研究领域: 材料科学 · 仿生学
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ACS Nano · 2024 · IF 15.8

Green Alga-Inspired Underwater Vision Based on Light-Driven Active Ion Transport across Janus Dual-Field Heterostructures

Lili Wang,Yuhui Zhang,Yupeng Chen,Lei Jiang

Natural organisms have evolved various biological ion channels to make timely responses toward different physical and/or chemical stimuli, giving guidance to construct artificial counterparts and expand the corresponding applications. They have also shown promising potential to overcome disadvantages of traditional electronic devices (e.g., energy-consuming operation and adverse humidity interference). Herein, we constructed a green alga-inspired nanofluidic system based on a Janus dual-field heterogeneous membrane (i.e., J-HM), which can function underwater as an artificial visual platform for light perception through enhanced active ion transport. The J-HM was obtained through sequentially assembled MXene and Cu-HHTP (i.e., a metal–organic framework based on the reaction between 2,3,6,7,10,11-hexahydroxytriphenylene hydrate (HHTP) and Cu2+) building units. Due to the formed temperature gradient and intramembrane electric field caused by the localized thermal excitation and efficient charge separation of J-HM under illumination, thermo-osmotic and photo-driven forces are generated for preferential cation transport from Cu-HHTP to MXene. Furthermore, unidirectional active transport can be enhanced by self-diffusion under a concentration gradient. Then, the corresponding underwater light perceptions at various light illumination conditions are explored, showing nearly a linear correlation with the light intensity. Finally, it is demonstrated that the visual platform can achieve object shape, definition, and distance recognition using a defined pixelated matrix, giving impetus to develop ionic signal transmission based sensing systems.

CAS / MDL: 7758-99-8
研究领域: 生物物理学 · 材料科学 · 仿生学
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES · 2024 ·Vol. 40 ·期 2 ·326-332 · IF 3.1

Outer-surface Covering of Nanochannels with Hydrogel for Highly Sensitive and Specific Cr(VI) Detection Through Analyte-caused Charge Change in Hydrogel

Liu Huan,Sun Xueting,Dai Yu,Zhang Xiaojin,Xia Fan

Nanochannels have made great progress and are a promising platform for detecting a series of targets. However, most nanochannels are modified on the inner wall, while ignoring the outer surface. Here, we modified the outer surface of nanochannels with hydrogel. Different from other reported outer-surface modification methods, we directly cover nanochannels with hydrogel to form heterogeneous membrane. The selected hydrogel hardly adsorbs other ions and shows specific adsorption for Cr(VI). The adsorption sites in hydrogel are homogeneous, and Cr(VI) adsorption onto hydrogel is endothermic and spontaneous. The charge in hydrogel changes after Cr(VI) adsorption, and the resulting current changes can be used for the detection of Cr(VI) with the detection limit of 10 −11 mol/L. Our platform is expected to be used for Cr(VI) detection in living organisms, especially within cells. This work provides a new approach for outer-surface modification of nanochannels and offers a new choice for nanochannel detection platforms.

研究领域: 纳米技术 · 分析化学 · 环境科学 · 生物传感器
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Interfacial Engineering of MXene-Based Heterogeneous Membranes with Enhanced Ion Selectivity in Vanadium Redox Flow Battery

Yanbo Zhang,Denghua Zhang,Qi Zhou,Xihao Zhang,Shaoyu Hou,Hongxiang He,Xiaoliang Wu,Quanlong Li,Jianguo Liu,Chuanwei Yan

Interfacial interactions profoundly influence the proton conductivity and ion selectivity of ion-exchange membranes. However, previous studies on membranes primarily focus on enhancing the selective-conductive properties of the secondary phase while neglecting interfacial regulation. In this study, PFSA/CF 3 SO 3 -M heterogeneous membrane is successfully fabricated by incorporating CF 3 SO 3 -M nanosheets—derived from organic Lewis acid (trifluoromethanesulfonic acid) etching of Ti 3 AlC 2 —into perfluorosulfonic acid resin (PFSA). Compared to PFSA/HF-M hybrid membrane containing fillers etched by inorganic acid (HF), the PFSA/CF 3 SO 3 -M heterogeneous membrane exhibits superior proton conductivity, reduces vanadium ion permeability, and the highest ion selectivity (11.7 S min cm −3 ) among all tested membranes. This enhancement arises from two mechanisms: the development of heterointerface proton transport channels between filler and PFSA matrix and the pH-responsive Donnan exclusion effect inherent to the filler. Electrochemical evaluations demonstrate that the PFSA/CF 3 SO 3 -M membrane outperforms conventional Nafion membrane in vanadium redox flow battery (VRFB) applications, achieving 98.1% coulombic efficiency and 84.2% energy efficiency after 800 cycles. Cost analysis reveals that the PFSA/CF 3 SO 3 -M heterogeneous membrane demonstrates a 59.8% reduction in membrane cost compared to Nafion 212 in a 2 MW × 6 h VRFB system. This work establishes an effective strategy for designing MXene-based ion-selective membranes through rational interfacial engineering.

CAS / MDL: 1493-13-6 196506-01-1
研究领域: 材料科学 · 电化学 · 膜技术 · 储能 · 化学工程
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BIOMATERIALS · 2022 · IF 15.304

A heterogenic membrane-based biomimetic hybrid nanoplatform for combining radiotherapy and immunotherapy against breast cancer

Pei Pan,Xue Dong,Ying Chen,Jing-Jie Ye,Yun-Xia Sun,Xian-Zheng Zhang

Radiotherapy is adopted to obliterate multiple malignant tumors clinically, which might also induce antitumor immune response. However, traditional radiotherapy is not enough to ablate tumors and activate long-term immunological response. Here, we developed a hybrid nanoplatform (MGTe) composed of GTe (glutathione (GSH) decorated Te nanoparticles) and fusing tumor cell membranes (TM) and bacterial outer membranes (BM). In this nanoplatform, GTe was designed for radiotherapy sensitization, concurrently the fusion of TM and BM was expected for amplifying antitumor immune. With a high-Z element, MGTe could enhance radiosensitivity by reactive oxygen species (ROS) production and cancer cell immunogenic death (ICD) under X-ray irradiation, which would also trigger antitumor immune. At meanwhile, TM and BM would further enlarge the immunological effects through antigen presenting cells (APCs) maturation and cytotoxic T lymphocytes (CTLs) stimulation. In this synergistic strategy, the combination of MGTe and X-ray showed significant tumor inhibition by radiation-driven immunotherapy, which will find great potential as an attractive clinical alternative to fight against tumor with reduced side effects.

研究领域: 肿瘤学 · 纳米技术 · 免疫学 · 放射生物学
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