Towards the direct instrumental identification of active electrocatalytic sites using scanning tunneling microscopy

使用扫描隧道显微镜直接仪器识别活性电催化位点

• 批准号: 320825100
• 负责人: Professor Dr. Aliaksandr Bandarenka
• 金额: --
• 依托单位: Arbeitsgruppe Physik der Energiewandlung und -Speicherung
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2016
• 资助国家: 德国
• 起止时间: 2015-12-31 至 2020-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/320825100?language=en
• 关键词: Towards; direct; instrumental; identification; active

A deeper understanding of complex objects of nature is not achievable without the development of new informative but at the same time affordable research tools, methodologies and procedures. Original and powerful approaches for probing and modeling will most likely remain pillars controlling the advances in materials science. In this project, we propose an approach for experimental identification of so-called active sites at the surface of heterogeneous electrocatalysts using electrochemical scanning tunneling microscopy. The project utilizes the basic idea that under reaction conditions the parameters defining the tunneling barrier over the catalytically active site in contact with liquid electrolytes will be different, and, importantly, vary with time (e.g. due to approaching reactants and/or departing products), compared to those over the inactive sites. Therefore, the tunneling current measured between the tip and the sample under potential control should also change with time in a different way revealing local processes. By comparing the tunneling current as a function of time and tip-to-surface distance over different surface sites, it would be possible to elucidate the location of the catalytic centers. Our preliminary results support this basic idea. Low-index and high-index single crystal electrodes with quasi-periodic surface structures and very low surface mobility of atoms, nanostructured systems, as well as catalytic reactions important for future sustainable energy provision will be used in this project as model objects and reactions, respectively. Quantum chemistry calculations will be used (in collaboration) to clearly reveal the underlying physical foundations of the method, to support the quantitative interpretation of the experimental data regarding the local catalytic activity, and to iteratively improve the methodology.

如果不开发新的信息丰富但同时又负担得起的研究工具、方法和程序，就无法更深入地了解复杂的自然物体。原始和强大的探测和建模方法很可能仍然是控制材料科学进步的支柱。在这个项目中，我们提出了一种方法，利用电化学扫描隧道显微镜在非均相电催化剂表面的所谓的活性位点的实验识别。该项目利用的基本思想是，在反应条件下，限定与液体电解质接触的催化活性位点上的隧穿势垒的参数与非活性位点上的参数相比将是不同的，并且重要的是，随时间变化（例如，由于接近的反应物和/或离开的产物）。因此，在电势控制下在尖端和样品之间测量的隧穿电流也应该以不同的方式随时间变化，从而揭示局部过程。通过比较隧道电流作为时间的函数和尖端到表面的距离在不同的表面站点，它将是可能的阐明的催化中心的位置。我们的初步结果支持这一基本观点。具有准周期性表面结构和极低表面原子迁移率的低折射率和高折射率单晶电极、纳米结构系统以及对未来可持续能源供应至关重要的催化反应将分别用作该项目的模型对象和反应。量子化学计算将用于（合作）清楚地揭示该方法的潜在物理基础，支持有关局部催化活性的实验数据的定量解释，并迭代改进该方法。

项目成果

Enhancing the Hydrogen Evolution Reaction Activity of Platinum Electrodes in Alkaline Media Using Nickel–Iron Clusters

• DOI: 10.1002/anie.202000383
• 发表时间: 2020-03
• 期刊: Angewandte Chemie (International Ed. in English)
• 作者: Song Xue;Richard W. Haid;Regina M. Kluge;Xing Ding;Batyr Garlyyev;J. Fichtner;Sebastian Watzele;Shujin Hou;A. Bandarenka

Revealing the nature of active sites in electrocatalysis

• DOI: 10.1039/c9sc02654a
• 发表时间: 2019-09-21
• 期刊: CHEMICAL SCIENCE
• 影响因子: 8.4
• 作者: Garlyyev, Batyr;Fichtner, Johannes;Calle-Vallejo, Federico
• 通讯作者: Calle-Vallejo, Federico

The nature of active centers catalyzing oxygen electro-reduction at platinum surfaces in alkaline media

• DOI: 10.1039/c8ee03228a
• 发表时间: 2019-01-01
• 期刊: ENERGY & ENVIRONMENTAL SCIENCE
• 影响因子: 32.5
• 作者: Liang, Yunchang;McLaughlin, David;Bandarenka, Aliaksandr S.
• 通讯作者: Bandarenka, Aliaksandr S.

In-situ visualization of hydrogen evolution sites on helium ion treated molybdenum dichalcogenides under reaction conditions

• DOI: 10.1038/s41699-019-0107-5
• 发表时间: 2019-07
• 期刊: npj 2D Materials and Applications
• 影响因子: 9.7
• 作者: E. Mitterreiter;Yunchang Liang;Matthias Golibrzuch;David McLaughlin;C. Csoklich;J. Bartl;A. Holleitner-A.-Ho

Engineering of Highly Active Silver Nanoparticles for Oxygen Electroreduction via Simultaneous Control over Their Shape and Size

• DOI: 10.1002/adsu.201700117
• 发表时间: 2017-12-01
• 期刊: ADVANCED SUSTAINABLE SYSTEMS
• 影响因子: 7.1
• 作者: Garlyyev, Batyr;Liang, Yunchang;Bandarenka, Aliaksandr S.
• 通讯作者: Bandarenka, Aliaksandr S.