Takács Dóra, Katana Bojana, Szerlauth Adél, Sebők Dániel, Tomšič Matija, Szilágyi István
MTA-SZTE Lendület Biocolloids Research Group, Department of Physical Chemistry and Materials Science, University of Szeged, 1 Rerrich Béla tér, H-6720 Szeged, Hungary.
Department of Applied and Environmental Chemistry, University of Szeged, 1 Rerrich Béla tér, H-6720 Szeged, Hungary.
Soft Matter. 2021 Oct 20;17(40):9116-9124. doi: 10.1039/d1sm01074c.
The influence of ionic liquid (IL) anions and cations on the charging and aggregation properties of layered double hydroxide (LDH) nanoparticles was systematically studied. Surface charge characteristics were explored using zeta potential measurements, while aggregation processes were followed in dynamic light scattering experiments in aqueous IL solutions. The results revealed that the aggregation rates of LDHs were sensitive to the composition of ILs leading to IL-dependent critical coagulation concentration (CCC) values being obtained. The origin of the interparticle forces was found to be electrostatic, in line with the classical Derjaguin-Landau-Verwey-Overbeek (DLVO) theory, as the experimental aggregation kinetics were in good agreement with the predicted data. The ion specific adsorption of IL anions led to different surface charge densities for LDHs, which decreased in the order Cl > Br > DCA > SCN > NO for counterions and BMIM > BMPYR > BMPY > BMPIP in the case of coions resulting in weaker electrical double layer repulsion in these sequences. Since van der Waals forces are always present and their strength does not depend significantly on the ionic strength, the CCC values decreased in the above order. The present results shed light on the importance of the interfacial arrangement of the IL constituent ions on the colloidal stability of particle dispersions and provide important information on the design of stable or unstable particle-ionic liquid systems.
系统研究了离子液体(IL)的阴离子和阳离子对层状双氢氧化物(LDH)纳米颗粒的带电和聚集性质的影响。使用zeta电位测量来探究表面电荷特性,同时在IL水溶液的动态光散射实验中跟踪聚集过程。结果表明,LDH的聚集速率对IL的组成敏感,从而得到了依赖于IL的临界凝聚浓度(CCC)值。发现粒子间作用力的起源是静电作用,这与经典的德亚金-朗道-韦弗-奥弗贝克(DLVO)理论一致,因为实验聚集动力学与预测数据吻合良好。IL阴离子的离子特异性吸附导致LDH具有不同的表面电荷密度,对于抗衡离子,表面电荷密度按Cl>Br>DCA>SCN>NO的顺序降低,对于共离子,表面电荷密度按BMIM>BMPYR>BMPY>BMPIP的顺序降低,导致这些序列中的双电层排斥力减弱。由于范德华力总是存在且其强度对离子强度的依赖性不显著,因此CCC值按上述顺序降低。目前的结果揭示了IL组成离子的界面排列对颗粒分散体胶体稳定性的重要性,并为稳定或不稳定的颗粒-离子液体系统的设计提供了重要信息。