Publication date: 28th August 2024
Fabricating halide perovskite-based electrodes for photo(electro)chemical (PEC) applications is challenging due to its complex multilayer device configuration, which consists of a top most protecting layer. The formation of pinholes in the protecting layer during synthesis can significantly limit the device stability [1]. Halide double perovskite (Cs2BIBIIIX6) single crystals offer distinct advantages over their nanocrystalline and polycrystalline counterparts, owing to a reduced number of structural defects, the absence of prevalent grain boundary, decreased charge carrier recombination, and improved charge carrier mobility as well as lifetime [2]. These properties place perovskite single crystals as promising candidates for PEC applications. While previous studies have explored the photoelectrochemical water oxidation of Cs2AgMCl6 stabilized in an acetonitrile and water (90:10) electrolyte with a pH of approximately 7 [3], the application of these single crystals for PEC has not yet been fully explored. Nonetheless, the oxygen evolution reaction (OER) mechanism under in situ conditions remains largely unexplored for these catalysts. In this work, the photoelectrochemical properties of Cs2AgMX6 single crystal photoanodes have been studied in an acetonitrile and water electrolyte for OER. Moreover, the OER mechanism is studied in in-situ conditions using scanning electrochemical microscopy (SECM) in feedback mode. Through SECM measurements, the local electrocatalytic activity is mapped at the centre and edges of the crystal facet via obtaining approach curves. This study sheds light on the designing of more efficient OER catalysts in the future.
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