具有串/并联复合离子输运特性的仿生纳米通道的构筑与整流性能

doi:10.7503/cjcu20180701

摘要/Abstract

摘要：

人工构筑了基于分枝氧化铝纳米通道的串/并联复合的纳流体二极管体系, 其具有可调的离子整流性能. 在这种两级分枝结构的1-2-2, 1-2-3, 1-3-2和1-3-3型氧化铝纳米通道中, 若将每一个分枝节点等效为一个二极管, 那么其一级分枝节点相当于串联的1个二极管, 二级分枝节点相当于并联的多个二极管. 因此1-2-2和1-2-3型纳米通道的电路图可等效为并联的2个二极管与第3个二极管相串联, 1-3-2和1-3-3型纳米通道的电路图可等效为并联的3个二极管与第4个二极管相串联. 但由于1-2-2和1-2-3型以及1-3-2和1-3-3型的二级分枝的结构和数目不同, 可将这4种纳米通道等效为不同的串/并联复合特性的纳流体二极管体系, 并且表现出依次增大的离子整流. 即分枝氧化铝纳米通道内部一级分枝和二级分枝的结构或数目共同调控的表面电荷非对称性可以改变其离子整流性能. 进一步地, 具有代表性的1-2-2型分枝纳米通道的整流率随分枝通道长度的增加而增加, 这表明分枝部分对整个串/并联复合纳流体二极管的整流特性起到决定性的作用. 相比于以前的单个离子二极管体系, 这种具有串/并联复合特性的多级分枝氧化铝纳米通道将为构筑更复杂的仿生纳流体二极管的研究提供有价值的借鉴.

关键词: 两级分枝氧化铝纳米通道, 串/并联复合特性, 纳流体二极管, 离子整流

Abstract:

Based on hierarchically branched alumina nanochannels, a serial/parallel composite nanofluidic diode system with experimentally adjustable ion rectification characteristics was fabricated. Using a simple anodization method, we fabricated four two-generation branched alumina nanochannels with 1-2-2, 1-2-3, 1-3-2 and 1-3-3 geometric structures. Among them, if we view each branch node as a diode, its first branch node will be equivalent to one series diode, and its second branch node will be equivalent to multiple parallel diodes. In this case, the circuits of the branched alumina nanochannels with 1-2-2 and 1-2-3 geometric structures are regarded as two parallel diodes and then the third diode in series. Similarly, the ones with 1-3-2 and 1-3-3 geometric structures are considered as three parallel diodes and then connected in series with the fourth diode. However, considering different structures and numbers of the secondary branches of the 1-2-2 and 1-2-3 alumina nanochannels as well as the 1-3-2 and 1-3-3 alumina nanochannels, the four branched alumina nanochannels will ultimately be classified into four nanofluidic diodes with serial/parallel composite characteristic. Accordingly, benefiting from cooperative asymmetry of the first-branched and the second-branched geometries, which affects the surface-charge distribution on inner walls, the branched alumina nanochannels with 1-2-2, 1-2-3, 1-3-2 and 1-3-3 structures exhibit gradually enhanced ionic rectification properties. Further, the rectification ratios of the representative 1-1-2 branched alumina nanochannels increase as the length of the branch channel increases. This indicates that the branch part with stronger ion selectivity plays a decisive role in the rectification characteristics of the entire series/parallel composite nanofluidic diode system. Compared with the previous single ion diode system, this serial/parallel composite nanofluidic diode with geometry-tailorable hierarchically branched alumina nanochannels could not only provide a basic platform to build ionic diode circuitry and more complex nanofluidic devices, but also spark further efforts to simulate the smart ion transport processes of multiple-channel with sparallel/serial mode in living bodies.

Key words: Hierarchically branched alumina nanochannel, Composite series/parallel characteristic, Nanofluidic diode, Ionic rectification

中图分类号:

O647

TrendMD:

张丹, 侯胜男, 刘友, 范霞. 具有串/并联复合离子输运特性的仿生纳米通道的构筑与整流性能. 高等学校化学学报, 2019, 40(5): 1019.

ZHANG Dan,HOU Shengnan,LIU You,FAN Xia. Fabrication and Rectification Studies of Serial/Parallel Composite Nanofluidic Diode Based on Hierarchically Branched Alumina Nanochannels^†. Chem. J. Chinese Universities, 2019, 40(5): 1019.

图/表 9

Fig.1 Schematic illustration for detection of ionic transport properties of two-generation branched alumina nanochannels with serial/parallel composite circuit characteristicsThe right figure in the dotted box is a schematic diagram of a representative single channel structure in the porous branched alumina nanochannels with 1-2-2 geometric structures.

Fig.2 Schematic diagram(left) and equivalent circuit component(right) of four kinds of representative single nanochannel belonging to the porous two-generation branched Al2O3 nanochannels with 1-2-2(A), 1-2-3(B), 1-3-2(C) and 1-3-3(D) geometric structures

Fig.3 SEM images of the cross-section(A1—D1), the first-generation(A2—D2) and second-generation(A3—D3) branched section and final opening ends(A4—D4) of four kinds of alumina nanochannels(A1—A4) 1-2-2; (B1—B4) 1-2-3; (C1—C4) 1-3-2; (D1—D4) 1-3-3.

Fig.4 SEM images of the primary opening ends of four kinds of porous alumina nanochannels at low(A) and high(B) resolution

Fig.5 Schematic illustration of pore diameters of the stem channels, first- and second-generation branched channels of porous alumina nanochannels

Fig.6 I-V properties(A) and ionic rectification ratios at ± 0.2 V(B) of two-generation branched alumina nanochannels with 1-2-2, 1-2-3, 1-3-2 and 1-3-3 geometric structures in 0.1 mmol/L KCl solution at pH=9.5

Fig.7 Schematic diagrams of representative single nanochannel in 1-2-2 branched alumina nanochannels with the total thickness of 30 μm(A) and 60 μm(B) of which stem length/branch length(Ds/Db) is about 2∶1(C), 1∶1(D) and 1∶2(E), respectively

Fig.8 Cross-sectional SEM images of 1-2-2 branched alumina nanochannels with the total thickness of 30 μm(A1—C1) and 60 μm(A2—C2)Stem length/branch length(Ds/Db): (A1, A2) 2∶1; (B1, B2) 1∶1; (C1, C2) 1∶2.

Fig.9 I-V properties of 1-2-2 branched alumina nanochannels with the total thickness of 30 μm(A) and 60 μm(B), and the corresponding ionic rectification ratios(C)

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