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离子门控通过致密碳纳米管膜的传输。

Gated ion transport through dense carbon nanotube membranes.

机构信息

Department of Chemical and Biological Engineering, University of Colorado, Boulder, Colorado 80309-0424, USA.

出版信息

J Am Chem Soc. 2010 Jun 23;132(24):8285-90. doi: 10.1021/ja9091769.

Abstract

Gated ion diffusion is found widely in hydrophobic biological nanopores, upon changes in ligand binding, temperature, transmembrane voltage, and mechanical stress. Because water is the main media for ion diffusion in these hydrophobic biological pores, ion diffusion behavior through these nanochannels is expected to be influenced significantly when water wettability in hydrophobic biological nanopores is sensitive and changes upon small external changes. Here, we report for the first time that ion diffusion through highly hydrophobic nanopores (approximately 3 nm) showed a gated behavior due to change of water wettability on hydrophobic surface upon small temperature change or ultrasound. Dense carbon nanotube (CNT) membranes with both 3-nm CNTs and 3-nm interstitial pores were prepared by a solvent evaporation process and used as a model system to investigate ion diffusion behavior. Ion diffusion through these membranes exhibited a gated behavior. The ion flux was turned on and off, apparently because the water wettability of CNTs changed. At 298 K, ion diffusion through dense CNT membranes stopped after a few hours, but it dramatically increased when the temperature was increased 20 K or the membrane was subjected to ultrasound. Likewise, water adsorption on dense CNT membranes increased dramatically at a water activity of 0.53 when the temperature increased from 293 to 306 K, indicating capillary condensation. Water adsorption isotherms of dense CNT membranes suggest that the adsorbed water forms a discontinuous phase at 293 K, but it probably forms a continuous layer, probably in the interstitial CNT regions, at higher temperatures. When the ion diffusion channel was opened by a temperature increase or ultrasound, ions diffused through the CNT membranes at a rate similar to bulk diffusion in water. This finding may have implications for using CNT membrane for desalination and water treatment.

摘要

门控离子扩散广泛存在于疏水性生物纳米孔中,其变化受到配体结合、温度、跨膜电压和机械应力的影响。由于水是这些疏水性生物孔中离子扩散的主要介质,因此当疏水性生物纳米孔中的润湿性对外部微小变化敏感并发生变化时,预计离子通过这些纳米通道的扩散行为将受到显著影响。在这里,我们首次报道,由于疏水性表面上水润湿性的变化,通过高度疏水性纳米孔(约 3nm)的离子扩散由于小的温度变化或超声而表现出门控行为。通过溶剂蒸发工艺制备了具有 3nm CNT 和 3nm 间孔隙的致密碳纳米管(CNT)膜,并将其用作模型系统来研究离子扩散行为。这些膜中的离子扩散表现出门控行为。离子通量被打开和关闭,显然是因为 CNT 的润湿性发生了变化。在 298K 时,致密 CNT 膜中的离子扩散在几个小时后停止,但当温度升高 20K 或膜受到超声时,其扩散显著增加。同样,当温度从 293 升高到 306K 时,致密 CNT 膜上水的活度为 0.53,水吸附急剧增加,表明发生了毛细凝结。致密 CNT 膜的水吸附等温线表明,在 293K 时,吸附水形成不连续相,但在较高温度下,它可能在 CNT 间隙区域形成连续层。当离子扩散通道通过温度升高或超声打开时,离子以类似于水中体相扩散的速率通过 CNT 膜扩散。这一发现可能对使用 CNT 膜进行脱盐和水处理具有重要意义。

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