Koizumi Ai, Tahara Hirofumi, Hirano Tomonori, Morita Akihiro
Department of Chemistry, Graduate School of Science , Tohoku University , Sendai 980-8578 , Japan.
Elements Strategy Initiative for Catalysts and Batteries (ESICB) , Kyoto University , Kyoto 615-8520 , Japan.
J Phys Chem Lett. 2020 Feb 20;11(4):1584-1588. doi: 10.1021/acs.jpclett.9b03742. Epub 2020 Feb 12.
Hard, hydrophilic ions that hardly transport over the water-oil interface by imposing external electric potential could undergo facile transport with a trace of ligand. Such phenomena, called "shuttling", are elucidated by microscopic investigation with molecular dynamics simulations. The catalytic role manifests itself in a 2-D free-energy surface within the nanometer range of the interface. The free-energy landscape clearly distinguishes the condition that the catalytic shuttling plays a vital role in the ion transport. The mechanism associated with transient complex formation at the interface is shown to be widely relevant to the ion kinetics and extends the conventional concept of facilitated ion transport.
通过施加外部电势很难在水油界面上传输的硬亲水性离子，在有微量配体的情况下可以轻松传输。这种被称为“穿梭”的现象通过分子动力学模拟的微观研究得到了阐明。催化作用在界面纳米范围内的二维自由能表面上表现出来。自由能景观清楚地区分了催化穿梭在离子传输中起关键作用的条件。结果表明，与界面处瞬态复合物形成相关的机制与离子动力学广泛相关，并扩展了促进离子传输的传统概念。
