In situ X-ray scattering studies of growth at liquid metal - liquid electrolyte interfaces

液态金属-液态电解质界面生长的原位 X 射线散射研究

• 批准号: 266661790
• 负责人: Professor Dr. Olaf Magnussen
• 金额: --
• 依托单位: Institut für Experimentelle und Angewandte Physik
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2014
• 资助国家: 德国
• 起止时间: 2013-12-31 至 2018-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/266661790?language=en
• 关键词: situ; ray; scattering; studies; growth

Growth at liquid-liquid interfaces is of substantial current interest for material synthesis. These fluid interfaces provide a soft, defect-free substrate and allow preparation of a wide range of different nanomaterials. Detailed understanding of phase formation processes at these interfaces is hampered by the lack of data on the atomic-scale interface structure and the underlying microscopic growth mechanisms. In this project we aim at fundamentally clarifying those for the specific case of electrochemically controlled growth at the interface between liquid metals (mercury, gallium) and aqueous electrolyte solutions using in situ X-ray scattering. First atomic scale data on such growth processes, obtained in our previous work for PbBrF at Hg electrodes, revealed a complex behavior, involving the formation of well-defined ultrathin crystalline precursor layers in between the two liquids. These serve as a template for the subsequent 3D crystal formation, leading to a quasi-epitaxial growth. In the proposed project we will systematically investigate the role of these phenomena in deposition processes at liquid metal - electrolyte interfaces as well as study the temporal evolution of the deposit morphology as a function of the employed potential. First, the growth of ionic compounds will be studied, employing lead halides as a model system. In particular, we will focus on the structure of the precursor layer as a function of halide species and liquid metal substrate and its role in steering the crystal growth. Secondly, we will investigate the growth of the semiconductor germanium at these interfaces by electrochemical liquid-liquid-solid deposition, a novel, technologically interesting process. Of particular importance here is clarification of the interface structure, the initial stages of growth, and the time-dependent morphology of the 3D deposit. As a part of these studies we will determine the atomic-scale structure of the Ga - electrolyte interface, specifically the potential- and temperature-dependent surface layering in the liquid metal, which in itself is an important topic. In addition, these experiments will help in further developing X-ray scattering methods as a tool for operando studies of growth processes at liquid-liquid interfaces.

液体液体界面的生长对于材料合成具有很大的当前利益。这些流体界面提供了无缺陷的底物，并允许制备各种不同的纳米材料。缺乏关于原子尺度界面结构和潜在的微观生长机制的数据，对这些接口处的相形过程的详细理解受到了阻碍。在这个项目中，我们旨在从根本上阐明使用原位X射线散射的液体金属（汞，凝胶​​）和水解溶液之间的电化学控制生长的特定情况。在我们先前针对HG电极的PBBRF工作中获得的此类生长过程的第一个原子量表显示出了复杂的行为，涉及两种液体之间定义明确定义的超薄晶体前体层。这些用作随后的3D晶体形成的模板，从而导致准截止日期生长。在拟议的项目中，我们将系统地研究这些现象在液态金属 - 电解质界面的沉积过程中的作用，并研究沉积物形态的时间演化，这是所采用潜力的函数。首先，将使用铅卤化物作为模型系统研究离子化合物的生长。特别是，我们将重点关注前体层的结构，这是卤化物物种和液态金属底物的函数及其在转向晶体生长中的作用。其次，我们将通过电化学液体液 - 固定沉积（这是一种新颖，技术上有趣的过程）来研究半导体锗在这些界面上的生长。这里特别重要的是阐明界面结构，生长的初始阶段以及3D沉积物的时间依赖性形态。作为这些研究的一部分，我们将确定GA-电解质界面的原子尺度结构，特别是液态金属中的潜在和温度依赖性表面分层，这本身就是一个重要的主题。此外，这些实验将有助于进一步开发X射线散射方法，作为在液体液体界面上对生长过程进行操作研究的工具。

项目成果

Temperature- and potential-dependent structure of the mercury-electrolyte interface

汞-电解质界面的温度和电位相关结构

• DOI: 10.1103/physrevb.93.165408
• 发表时间: 2016
• 期刊: Physical Review B
• 影响因子: 3.7
• 作者: B. Runge;S. Festersen;C.T. Koops;A. Elsen;M. Deutsch;B.M. Ocko;O.H. Seeck;B.M. Murphy;O.M. Magnussen
• 通讯作者: O.M. Magnussen

The Atomic scale structure of liquid metal-electrolyte interfaces.

液态金属-电解质界面的原子尺度结构

• DOI: 10.1039/c6nr01571a
• 发表时间: 2016
• 期刊: Nanoscale
• 影响因子: 6.7
• 作者: B.M. Murphy;S. Festersen;O.M. Magnussen
• 通讯作者: O.M. Magnussen

X-ray reflectivity from curved liquid interfaces.

弯曲液体界面的 X 射线反射率

• DOI: 10.1107/s1600577517018057
• 发表时间: 2018
• 期刊: Journal of synchrotron radiation
• 影响因子: 2.5
• 作者: S. Festersen;S.B. Hrkac;C.T. KoopsB. Runge;T. Dane;B.M. Murphy;O.M. Magnussen
• 通讯作者: O.M. Magnussen