Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
DOI: https://doi.org/10.29363/nanoge.matsusfall.2024.077
Publication date: 28th August 2024
Among the various strategies proposed for enhancing the photoelectrochemical (PEC) performance of state-of-the-art photoelectrodes, the construction of heterostructures based on semiconductors and co-catalysts is widely acknowledged as one of the most versatile and reliable. This approach is often associated with higher quantum efficiency for photoinduced redox processes, due to improved interfacial charge transfer dynamics, and reduced degradation due to photocorrosion, as the photoinduced charge is less susceptible to this less competitive pathway. However, numerous studies[1-3] have demonstrated that this simplistic view conceals a much more complex microscopic nature, often significantly dependent on the specific characteristics of the interfaces. Therefore, understanding the redox dynamics in such complex systems is essential to direct the carriers along the desired pathways. Several indirect methods are available for this purpose, such as electrochemical impedance spectroscopy (EIS) and transient absorption spectroscopy (TAS), but operando X-ray absorption spectroscopy (XAS) stands out as the most promising technique[4,5]. Operando XAS can provide direct, element-selective information about changes in the redox state and the local environment of the co-catalyst metal centers.
In line with this aim, we report our recent advancements in the development of operando PEC-XAS experimental techniques to understand the redox dynamics of various semiconductor/co-catalyst assemblies, fully replicating the operating conditions of a PEC cell. This tool is employed to investigate potential and light-induced processes in i) BiVO4/WO3 heterostructures coated with Co-based co-catalysts, providing evidence for specific electronic interactions with the semiconductor, and ii) Ni-based co-catalysts on hematite photoanodes, offering insights into the rate-determining step of PEC oxidation of biomass derivatives by such systems. Additionally, operando PEC-XAS has proven to be an invaluable tool for monitoring degradation processes, as it enables structural understanding and real-time monitoring of the dissolution processes of the catalysts' active elements.
We gratefuly acknowledge the European Union’s Horizon 2020 research and innovation programme, under Grant No. 101006839 (H2020 Research Innovation Actions
2020-2024 “CONDOR”), and the Italian Minister of University and Research, under PRIN 2022 2022Z8RM7C "Electro- and Photoelectro-chemical CO2 conversion in eXtreme environments - EPiCX".
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