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Effect of Pore Connectivity on the Behavior of Fluids Confined in Sub-Nanometer Pores: Ethane and CO

机译:孔隙连通性对亚纳米毛孔中狭窄的流体行为的影响:乙烷与CO

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摘要

The behavior of fluids under nano-confinement varies from that in bulk due to an interplay of several factors including pore connectivity. In this work, we use molecular dynamics simulations to study the behavior of two fluids—ethane and CO2 confined in ZSM-22, a zeolite with channel-like pores of diameter 0.55 nm isolated from each other. By comparing the behavior of the two fluids in ZSM-22 with that reported earlier in ZSM-5, a zeolite with pores of similar shape and size connected to each other via sinusoidal pores running perpendicular to them, we reveal the important role of pore connectivity. Further, by artificially imposing pore connectivity in ZSM-22 via inserting a 2-dimensional slab-like inter-crystalline space of thickness 0.5 nm, we also studied the effect of the dimensionality and geometry of pore connectivity. While the translational motion of both ethane and CO2 in ZSM-22 is suppressed as a result of connecting the pores by perpendicular quasi-one-dimensional pores of similar dimensions, the effect of connecting the pores by inserting the inter-crystalline space is different on the translational motion of the two fluids. For ethane, pores connected via inter-crystalline space facilitate translational motion but suppress rotational motion, whereas in the case of CO2, both types of motion are suppressed by pore connection due to the strong interaction of CO2 with the surface of the substrate.
机译:由于几种因素在内的孔连接,因此纳米限制下的流体的行为因散装而异。在这项工作中,我们使用分子动力学模拟来研究两个流体 - 乙烷和二氧化碳局限于ZSM-22中的沸石的行为,具有彼此分离的通道状孔的沸石。通过比较ZSM-22中的两个流体的行为,在ZSM-5之前报道,沸石通过垂直于它们的正弦孔彼此相互连接的类似形状和尺寸的沸石,我们揭示了孔连接的重要作用。此外,通过将ZSM-22中的孔隙连接通过插入厚度为0.5nm的二维板状晶间空间,通过在ZSM-22中呈现孔隙连通性,我们还研究了孔连接的维度和几何形状的效果。虽然ZSM-22中的乙烷和二氧化碳的平移运动被抑制由于相似尺寸的垂直准一维孔连接孔,但通过插入晶间空间通过插入晶体间隔的效果是不同的两种流体的平移运动。对于乙烷,通过晶间空间连接的孔促进平移运动但抑制旋转运动,而在CO2的情况下,由于CO2与基板表面的强的相互作用,通过孔连接抑制两种运动。

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