Lobel Benjamin T, Baiocco Daniele, Al-Sharabi Mohammed, Routh Alexander F, Zhang Zhibing, Cayre Olivier J
School of Chemical and Process Engineering, University of Leeds, Leeds, LS2 9JT, United Kingdom.
School of Chemical Engineering, University of Birmingham, Birmingham, B15 2TT, United Kingdom.
Langmuir. 2025 Jan 14;41(1):550-562. doi: 10.1021/acs.langmuir.4c03812. Epub 2024 Dec 26.
To form nonspherical emulsion droplets, the interfacial tension driving droplet sphericity must be overcome. This can be achieved through interfacial particle jamming; however, careful control of particle coverage is required. In this work, we present a scalable novel batch process to form nonspherical particle-stabilized emulsions. This is achieved by concurrently forming interfacially active particles and drastically accelerating emulsion destabilization through addition of electrolyte. To achieve this, surfactant-stabilized oil-in-water emulsions in the presence of dopamine were first produced. These emulsions were then treated with tris(hydroxymethyl)aminomethane hydrochloride buffer to both simultaneously initiate polymerization of dopamine in the emulsion continuous phase and reduce the Debye length of the system, thus accelerating droplet coalescence while forming surface-active particles. The concentration of buffer and imposed shear was then systematically varied, and the behavior at the interface was studied using pendent drop tensiometry and interfacial shear rheology. It was found that polydopamine nanoparticles formed in the emulsion continuous phase adsorbed to the reducing interface during coalescence, resulting in anisotropic droplets formed via arrested coalescence. Greater shear rates resulted in accelerated coalescence and formation of secondary droplets, whereas lower shear rates resulted in thicker interfacial films. The efficacy of this method was further demonstrated with a second system consisting of sodium dodecyl sulfate as the surfactant and polypyrrole particles, which also resulted in nonspherical droplets for optimized conditions.
为了形成非球形乳液液滴,必须克服驱动液滴呈球形的界面张力。这可以通过界面颗粒堵塞来实现;然而,需要仔细控制颗粒覆盖率。在这项工作中,我们提出了一种可扩展的新型间歇工艺来形成非球形颗粒稳定乳液。这是通过同时形成界面活性颗粒并通过添加电解质大幅加速乳液失稳来实现的。为了实现这一点,首先制备了在多巴胺存在下由表面活性剂稳定的水包油乳液。然后用三(羟甲基)氨基甲烷盐酸盐缓冲液处理这些乳液,以同时引发乳液连续相中多巴胺的聚合,并减小体系的德拜长度,从而在形成表面活性颗粒的同时加速液滴聚结。然后系统地改变缓冲液浓度和施加的剪切力,并使用悬滴张力测量法和界面剪切流变学研究界面处的行为。结果发现,在乳液连续相中形成的聚多巴胺纳米颗粒在聚结过程中吸附到还原界面上,导致通过聚结停滞形成各向异性液滴。较高的剪切速率导致聚结加速和二次液滴的形成,而较低的剪切速率导致界面膜变厚。该方法的有效性在第二个系统中得到了进一步证明,该系统由十二烷基硫酸钠作为表面活性剂和聚吡咯颗粒组成,在优化条件下也产生了非球形液滴。