Wu Jiedu, Liu Shuai, Tan Zhuo, Guo Yuting, Zhou Jianzhang, Mao Bingwei, Yan Jiawei
State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian 361005, People's Republic of China.
J Chem Phys. 2021 Dec 28;155(24):244702. doi: 10.1063/5.0073792.
Choline chloride (ChCl)-based-deep eutectic solvents (DESs) are widely used in electrochemical fields. In this work, the effect of two types of hydrogen bond donor (HBD) molecules, ethylene glycerol and lactic acid (LA), on electrochemical interfaces between the Au electrode and DESs has been investigated by employing voltammetry and electrochemical impedance spectroscopy. The anodic dissolution and passivation behaviors of the Au electrode are revealed in both ethaline and ChCl:LA. In ChCl:LA, the anodic dissolution of Au is slowed down, and the passivation film is relatively dense and stable due to the existence of the carboxyl group in HBD molecule LA. In the double layer region, the lifting and formation of Au(111) surface reconstruction and a disorder-order phase transition of the chloride ion adlayer were observed in the two DESs. Moreover, compared with ethaline, an extra pair of current peaks appears in ChCl-LA possibly due to the adsorption and desorption of LA on the Au(111) surface, which might imply the stronger interaction of LA with the Au electrode in ChCl:LA. HBD LA could even have marked an impact on the disorder-order phase transition of the chloride ion adlayer. The above results provide new insight into the significant effect of HBD molecules on the anodic dissolution and the passivation of the Au electrode and the electrochemical behaviors in the double layer region.
基于氯化胆碱(ChCl)的深共熔溶剂(DESs)在电化学领域得到了广泛应用。在本工作中,通过伏安法和电化学阻抗谱研究了两种氢键供体(HBD)分子,即乙二醇和乳酸(LA),对金电极与DESs之间电化学界面的影响。在乙酰胺和ChCl:LA中均揭示了金电极的阳极溶解和钝化行为。在ChCl:LA中,由于HBD分子LA中羧基的存在,金的阳极溶解减缓,钝化膜相对致密且稳定。在双层区域,在两种DESs中均观察到了Au(111)表面重构的起伏和形成以及氯离子吸附层的无序-有序相变。此外,与乙酰胺相比,ChCl-LA中出现了额外的一对电流峰,这可能是由于LA在Au(111)表面的吸附和解吸,这可能意味着LA与ChCl:LA中的金电极相互作用更强。HBD LA甚至可能对氯离子吸附层的无序-有序相变产生显著影响。上述结果为HBD分子对金电极的阳极溶解和钝化以及双层区域电化学行为的显著影响提供了新的见解。