Papaderakis Athanasios A, Polus Kacper, Kant Pallav, Box Finn, Etcheverry Bruno, Byrne Conor, Quinn Martin, Walton Alex, Juel Anne, Dryfe Robert A W
Department of Chemistry, University of Manchester, Oxford Road, ManchesterM13 9PL, United Kingdom.
Henry Royce Institute, University of Manchester, Oxford Road, ManchesterM13 9PL, United Kingdom.
J Phys Chem C Nanomater Interfaces. 2022 Dec 15;126(49):21071-21083. doi: 10.1021/acs.jpcc.2c06517. Epub 2022 Nov 30.
Wetting of carbon surfaces is one of the most widespread, yet poorly understood, physical phenomena. Control over wetting properties underpins the operation of aqueous energy-storage devices and carbon-based filtration systems. Electrowetting, the variation in the contact angle with an applied potential, is the most straightforward way of introducing control over wetting. Here, we study electrowetting directly on graphitic surfaces with the use of aqueous electrolytes to show that reversible control of wetting can be achieved and quantitatively understood using models of the interfacial capacitance. We manifest that the use of highly concentrated aqueous electrolytes induces a fully symmetric and reversible wetting behavior without degradation of the substrate within the unprecedented potential window of 2.8 V. We demonstrate where the classical "Young-Lippmann" models apply, and break down, and discuss reasons for the latter, establishing relations among the applied bias, the electrolyte concentration, and the resultant contact angle. The approach is extended to electrowetting at the liquid|liquid interface, where a concentrated aqueous electrolyte drives reversibly the electrowetting response of an insulating organic phase with a significantly decreased potential threshold. In summary, this study highlights the beneficial effect of highly concentrated aqueous electrolytes on the electrowettability of carbon surfaces, being directly related to the performance of carbon-based aqueous energy-storage systems and electronic and microfluidic devices.
碳表面的润湿性是最为普遍但却了解甚少的物理现象之一。对润湿性的控制是水系储能装置和碳基过滤系统运行的基础。电润湿,即接触角随外加电势的变化,是实现对润湿性进行控制的最直接方式。在此,我们利用水性电解质直接研究石墨表面的电润湿现象,结果表明,借助界面电容模型能够实现对润湿性的可逆控制并进行定量理解。我们证明,在2.8 V这一前所未有的电势窗口内,使用高浓度水性电解质可诱导出完全对称且可逆的润湿行为,同时不会使基底降解。我们展示了经典的“杨氏-利普曼”模型适用和失效的情况,并讨论了后者的原因,确立了外加偏压、电解质浓度与所得接触角之间的关系。该方法被扩展至液-液界面的电润湿,在此情况下,高浓度水性电解质能以显著降低的电势阈值可逆地驱动绝缘有机相的电润湿响应。总之,本研究突出了高浓度水性电解质对碳表面电润湿性的有益影响,这与碳基水系储能系统以及电子和微流控装置的性能直接相关。