Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.190
Publication date: 18th December 2023
The chemical instability of halide perovskites (HaP) in protic solvents remains the main obstacle to their utilization in photoelectrochemical devices. Despite the implementation of protective strategies for PEC applications[1], [2], systematic studies of (photo)electrochemical processes and the potential corrosion of perovskite/electrolyte interfaces and their impact on energy conversion and stability are still lacking [3].
In this study, we examined the photoelectrochemical behavior of 2D di-phenylethylammonium lead tetra iodide (PEAH2PbI4) thin films as a model system to study fundamental photoelectrochemical processes of metal halide perovskites. We found the use of excess PEAI in solution necessary to stabilize the thin films like by chemical equilibrium and a surfactant effect. Introducing the Fe(CN)6 3-/4- redox couple electroactive species and considering PEAI a supporting electrolyte and stabilization agent [4],[5], we studied photo-electrochemical processes at the semiconductor/electrolyte interface by monitoring the open-circuit potential (OCP). Under illumination, a potential inversion was observed for different equilibrium concentrations of the redox probe. In-situ UV-Vis and XRD analyses provided compelling evidence indicating that the potential inversion, indicating either electron or hole accumulation on the PEAH2PbI4, leads to different photo-corrosion phenomena. Lead iodide, PbI2, as well as a phenylethylamine-lead iodide intercalation compound, (PEA)-PbI2 , are observed as degradation products. Surface photovoltage (SPV) studies revealed that the redox probe ratio determines carrier separation dynamics at the 2D perovskite / electrolyte interface. Based on the SPV results, we conclude that electron transfer to the redox couple is a critical step in suppressing photodegradation of the material in aqueous solutions. These findings shed light on the intricate interplay between carrier dynamics and chemical changes in the context of semiconductor/electrolyte interfaces, providing valuable insights for the development of design strategies to effectively utilize halide perovskites as photoelectrodes. In addition, our findings provide fundamental insight into the photo-corrosion processes of HaPs, which are currently of high interest for many applications foremost solar cells.
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