Jellicoe Matt, Igder Aghil, Chuah Clarence, Jones Darryl B, Luo Xuan, Stubbs Keith A, Crawley Emily M, Pye Scott J, Joseph Nikita, Vimalananthan Kasturi, Gardner Zoe, Harvey David P, Chen Xianjue, Salvemini Filomena, He Shan, Zhang Wei, Chalker Justin M, Quinton Jamie S, Tang Youhong, Raston Colin L
Flinders Institute for Nanoscale Science and Technology, College of Science and Engineering, Flinders University Bedford Park SA 5042 Australia
School of Molecular Sciences, The University of Western Australia 35 Stirling Highway Crawley WA 6009 Australia.
Chem Sci. 2022 Jan 31;13(12):3375-3385. doi: 10.1039/d1sc05829k. eCollection 2022 Mar 24.
Mixing immiscible liquids typically requires the use of auxiliary substances including phase transfer catalysts, microgels, surfactants, complex polymers and nano-particles and/or micromixers. Centrifugally separated immiscible liquids of different densities in a 45° tilted rotating tube offer scope for avoiding their use. Micron to submicron size topological flow regimes in the thin films induce high inter-phase mass transfer depending on the nature of the two liquids. A hemispherical base tube creates a Coriolis force as a 'spinning top' (ST) topological fluid flow in the less dense liquid which penetrates the denser layer of liquid, delivering liquid from the upper layer through the lower layer to the surface of the tube with the thickness of the layers determined using neutron imaging. Similarly, double helical (DH) topological flow in the less dense liquid, arising from Faraday wave eddy currents twisted by Coriolis forces, impact through the less dense liquid onto the surface of the tube. The lateral dimensions of these topological flows have been determined using 'molecular drilling' impacting on a thin layer of polysulfone on the surface of the tube and self-assembly of nanoparticles at the interface of the two liquids. At high rotation speeds, DH flow also occurs in the denser layer, with a critical rotational speed reached resulting in rapid phase demixing of preformed emulsions of two immiscible liquids. ST flow is perturbed relative to double helical flow by changing the shape of the base of the tube while maintaining high mass transfer between phases as demonstrated by circumventing the need for phase transfer catalysts. The findings presented here have implications for overcoming mass transfer limitations at interfaces of liquids, and provide new methods for extractions and separation science, and avoiding the formation of emulsions.
混合互不相溶的液体通常需要使用辅助物质,包括相转移催化剂、微凝胶、表面活性剂、复合聚合物和纳米颗粒以及/或者微混合器。在一个倾斜45°的旋转管中对不同密度的互不相溶液体进行离心分离,为避免使用这些辅助物质提供了可能。薄膜中微米到亚微米尺寸的拓扑流动状态会根据两种液体的性质引发高效的相间传质。一个半球形底管会产生科里奥利力,形成一种“陀螺”(ST)拓扑流体流,存在于密度较小的液体中,该流体流会穿透密度较大的液层,将上层液体通过下层输送到管的表面,液层厚度通过中子成像确定。同样地,密度较小的液体中由科里奥利力扭曲的法拉第波涡流产生的双螺旋(DH)拓扑流,会通过密度较小的液体冲击到管的表面。这些拓扑流的横向尺寸已通过“分子钻孔”确定,“分子钻孔”作用于管表面的聚砜薄层,以及通过纳米颗粒在两种液体界面处的自组装来确定。在高转速下,DH流也会出现在密度较大的液层中,当达到临界转速时,会导致两种互不相溶液体的预制乳液快速相分离。通过改变管底部的形状,相对于双螺旋流而言,ST流会受到扰动,同时各相之间仍保持高效传质,这一点通过无需相转移催化剂得以证明。此处呈现的研究结果对于克服液体界面处的传质限制具有重要意义,并为萃取和分离科学提供了新方法,同时避免乳液的形成。