Han Junghyup, Yoon Sun Geun, Lee Won Hyung, Jin Huding, Cho Yong Hyun, Kim Youn Sang
School of Chemical and Biological Engineering, and Institute of Chemical Processes, College of Engineering, Seoul National University, Gwanak-gu, Seoul, 08826, Republic of Korea.
Program in Nano Science and Technology, Graduate School of Convergence Science and Technology, Seoul National University, Gwanak-gu, Seoul, 08826, Republic of Korea.
Adv Sci (Weinh). 2022 Jan;9(1):e2103038. doi: 10.1002/advs.202103038. Epub 2021 Oct 31.
Ion-solid surface interactions are one of the fundamental principles in liquid-interfacing devices ranging from various electrochemical systems to electrolyte-driven energy conversion devices. The interplays between these two phases, especially containing charge carriers in the solid layer, work as a pivotal role in the operation of these devices, but corresponding details of those effects remain as unrevealed issues in academic fields. Herein, an ion-charge carrier interaction at an electrolyte-semiconductor interface is interrogated with an ion-dynamics-induced (ionovoltaic) energy transducer, controlled by interfacial self-assembled molecules. An electricity generating mechanism from interfacial ionic diffusion is elucidated in terms of the ion-charge carrier interaction, originated from a dipole potential effect of the self-assembled molecular layer (SAM). In addition, this effect is found to be modulated via chemical functionalization of the interfacial molecular layer and transition metal ion complexation therein. With the aiding of surface analytic techniques and a liquid-interfacing Hall measurement, electrical behaviors of the device depending on the magnitude of the ion-ligand complexation are interrogated, thereby demonstrating the ion-charge carrier interplays spanning at electrolyte-SAM-semiconductor interface. Hence, this system can be applied to study molecular interactions, including chemical and physical influences, occurring at the solid-liquid interfacial region.
离子与固体表面的相互作用是从各种电化学系统到电解质驱动的能量转换装置等液体界面装置的基本原理之一。这两个相之间的相互作用，特别是固体层中包含电荷载流子的情况，在这些装置的运行中起着关键作用，但这些效应的相应细节在学术领域仍是未揭示的问题。在此，利用由界面自组装分子控制的离子动力学诱导（离子光伏）能量换能器研究电解质 - 半导体界面处的离子 - 电荷载流子相互作用。根据离子 - 电荷载流子相互作用阐明了界面离子扩散产生电能的机制，该相互作用源于自组装分子层（SAM）的偶极电势效应。此外，发现这种效应可通过界面分子层的化学功能化及其内过渡金属离子络合进行调节。借助表面分析技术和液体界面霍尔测量，研究了装置的电学行为与离子 - 配体络合强度的关系，从而证明了跨越电解质 - SAM - 半导体界面的离子 - 电荷载流子相互作用。因此，该系统可用于研究在固液界面区域发生的分子相互作用，包括化学和物理影响。
