Aqueous proton-selective conduction across two-dimensional graphyne
Aqueous proton-selective conduction across two-dimensional graphyne
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DOI：
10.1038/s41467-019-09151-8
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发表时间：
2019-03
影响因子：
16.6
通讯作者：
Le Shi;Ao Xu;D. Pan;T. Zhao
中科院分区：
文献类型：
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作者：
Le Shi;Ao Xu;D. Pan;T. Zhao
直接甲醇燃料电池的发展受到甲醇跨膜渗透问题的阻碍，尽管使用液体燃料产生了显着的功能。在这里，我们调查质子选择性导电行为在2D石墨在水环境中。当三角形石墨炔孔的边长增加到0.95 nm时，水溶液的质子传导机制从裸质子穿透过渡到混合的车辆和Grotthuss运输。边长进一步增加到1.2 nm导致图案化的水/真空界面的形成，使得质子能够通过具有低能量势垒的Grotthuss机制传导通过水线。更重要的是，发现边长小于1.45 nm的2D石墨炔可以有效地阻止甲醇渗透，这表明具有适当孔径的2D石墨炔是实现零渗透质子选择性膜的理想材料。
The development of direct methanol fuel cells is hindered by the issue of methanol crossover across membranes, despite the remarkable features resulting from the use of liquid fuel. Here we investigate the proton-selective conduction behavior across 2D graphyne in an aqueous environment. The aqueous proton conduction mechanism transitions from bare proton penetration to a mixed vehicular and Grotthuss transportation when the side length of triangular graphyne pores increases to 0.95 nm. A further increase in the side length to 1.2 nm results in the formation of a patterned aqueous/vacuum interphase, enabling protons to be conducted through the water wires via Grotthuss mechanism with low energy barriers. More importantly, it is found that 2D graphyne with the side length of less than 1.45 nm can effectively block methanol crossover, suggesting that 2D graphyne with an appropriate pore size is an ideal material to achieve zero-crossover proton-selective membranes.