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Quantifying and Decoupling Molecular Interactions of Ionic Liquids with Gold Electrodes.

Xin WangQingwei GaoLicheng LiGaurav TatrariFaiz Ullah ShahAatto LaaksonenXiaoyan JiRong An
Published in: Langmuir : the ACS journal of surfaces and colloids (2024)
This work combined gold colloid probe atomic force microscopy (AFM) with a quartz crystal microbalance (QCM) to accurately quantify the molecular interactions of fluorine-free phosphonium-based ionic liquids (ILs) with gold electrode surfaces. First, the interactions of ILs with the gold electrode per unit area ( F A ' , N/m 2 ) were obtained via the force-distance curves measured by gold probe AFM. Second, a QCM was employed to detect the IL amount to acquire the equilibrium number of IL molecules adsorbed onto the gold electrode per unit area ( N IL , Num/m 2 ). Finally, the quantified molecular interactions of ILs with the gold electrode ( F 0 , nN/Num) were estimated. F 0 is closely related to the IL composition, in which the IL with the same anion but a longer phosphonium cation exhibits a stronger molecular interaction. The changes in the quantified interactions of gold with different ILs are consistent with the interactions predicted by the extended Derjaguin-Landau-Verwey-Overbeek theory, and the van der Waals interaction was identified as the major contribution of the overall interaction. The quantified molecular interaction is expected to enable the direct experimental-derived interaction parameters for molecular simulations and provide the virtual design of novel ILs for energy storage applications.
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