论文标题

通过分子薄膜的气体传输机制

Gas transport mechanisms through molecularly thin membranes

论文作者

Stroganov, Vladislav, Hüger, Daniel, Neumann, Christof, Noethel, Tabata, Steinert, Michael, Huebner, Uwe, Turchanin, Andrey

论文摘要

具有内在的亚纳米孔隙率的原子薄分子碳纳米膜(CNM)被认为是下一代过滤和气体分离应用的有前途的候选物,由于其厚度极低,能量效率和选择性。 CNM是本质上多孔的,比其他2D材料(例如石墨烯和过渡金属二核苷)具有优势,在合成后需要引入缺陷和毛孔。已经发现,水和氦气通过检测极限以上的4,4-二苯基硫醇(TPT)CNM渗透。此外,尽管它们的动力学直径相似,但水蒸气的渗透是非线性的,并且比氦气的渗透性强1000。但是,没有明显的渗透机制可以解释这两种物种的渗透。在这里,我们证明了所有气体物种的渗透是由它们的吸附来定义的。我们在不同温度下通过TPT CNM进行了气体渗透测量,发现所有测量的气体均具有与动力学直径相关的激活能屏障。此外,我们确定在吸附和渗透过程中的熵损失是强烈非线性渗透水的基本原因。我们的结果还表明,吸附在所有气体的渗透中起着重要作用,而不仅仅是水。

Atomically thin molecular carbon nanomembranes (CNMs) with intrinsic sub-nanometer porosity are considered as promising candidates for next generation filtration and gas separation applications due to their extremely low thickness, energy efficiency and selectivity. CNMs are intrinsically porous which is advantageous over other 2D materials such as graphene and transition metal dichalcogenides where defects and pores need to be introduced after synthesis. It was already discovered that water and helium permeate through 4,4-terphenylthiol (TPT) CNM above the limit of detection. Additionally, the permeation of water vapour was nonlinear against its pressure and 1000 stronger than permeation of helium despite their similar kinetic diameters. However, there was no clear permeation mechanism which could explain permeation of both species. Here, we demonstrate that permeation of all gas species is defined by their adsorption. We performed gas permeation measurements through TPT CNM at different temperatures and found that all measured gases experienced an activation energy barrier which correlated with their kinetic diameters. Furthermore, we identified that entropy loss during adsorption and permeation is the fundamental reason of strong nonlinear permeation of water. Our results also demonstrated that adsorption plays a major role in permeation of all gases, not just water.

扫码加入交流群

加入微信交流群

微信交流群二维码

扫码加入学术交流群,获取更多资源