Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.167
Publication date: 18th July 2023
A fundamental understanding of processes occurring at the electrode-electrolyte interface is essential for the development of optimized materials in sustainable energy production. In this talk, I will present two examples that highlight the relevance of atomistic studies on model electrocatalytic systems in understanding existing structure-function relationships and reaction-mechanism.
Firstly, I will introduce our custom experimental setup, which enables a comprehensive characterization of structural, chemical, and electrochemical properties on the same sample. This setup facilitates the transfer of electrodes from ultra-high vacuum conditions, ideal for surface science tools, to an electrochemical cell in an inert atmosphere. By employing this approach, we investigated potential-induced changes on Au(111) surfaces in acidic media. We monitored chemical transformations using ex-situ X-ray photoemission spectroscopy (XPS), providing insights into the electrochemical response, including oxide formation during the onset of the oxygen evolution reaction. Additionally, I will discuss the influence of various electrolyte anions on surface electro-oxidation.
Secondly, I will provide an overview of the local properties of point defects in transition metal dichalcogenide semiconductors (MX2, M = transition metal, X = chalcogen) that have been proposed as active sites for the hydrogen evolution reaction (HER). By combining 4K scanning tunneling microscopy and spectroscopy (STM/STS), and non-contact atomic force microscopy (nc-AFM), we achieved atomic-scale correlation between the morphology and electronic properties of different types of structural defects in MoSe2 and WS2 monolayers. Our investigations unveiled the predominance of substitutional oxygen as the point defect in these semiconductors, effectively suppressing deep in-gap states associated with chalcogen vacancies [1, 2], which have been discussed to mediate the HER. These findings highlight the critical role of local properties in determining the functionality of materials for hydrogen production, ultimately governing the underlying reaction mechanism.
Work supported by grants PID2020-116093RB-C44, EUR2020-112066 & RYC-2017-21931 funded by MCIN/AEI /10.13039/501100011033 and European Union NextGenerationEU/PRTR and by ESF Investing in your future.
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