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Organic–inorganic hybrid perovskites are widely utilized in solar driven chemistry such as photocatalysis, hydrogen evolution, and oxygen reduction. Hybrid perovskites contain various components with high polarity and/or charge values, which undergo transformations due to ion exchange, photoinduced phase segregation, or ion migration. These variable characteristics make perovskites "soft materials". Meanwhile, optoelectronic devices often operate under electrochemical reactions in the presence of an electrical field. To examine the effect of this field on the material/photophysical properties of hybrid perovskites, hybrid FAPbBr3 (FA+: CH(NH2)2+) perovskite quantum dots (PQDs) were synthesized. In this study, we report the spectroelectrochemical investigation of the hybrid FAPbBr3 PQDs to understand the electrochemical stability and degradation process. We also found that the electrochemical condition played an important role in inducing defect-mediated oxidation/reduction reactions, changing the photophysical properties of hybrid PQDs, and causing their irreversible transformations to various lead halide plumbate complexes. These findings can help develop a strategy for enhancing the operational performance of PQDs for the solar driven chemistry. [ABSTRACT FROM AUTHOR]

Making high-quality raw materials is the key to open the versatile potential of next generation materials. All-inorganic CsPbX3 (X: Cl−, Br−, and/or I−) perovskite quantum dots (PQDs) have been applied in various optoelectronic devices, such as photocatalysis, hydrogen evolution, solar cells, and light-emitting diodes, due to their outstanding photophysical properties, such as high photoluminescence quantum yield (PLQY), absorption cross-section, efficient charge separation, and so on. Specifically, for further improvement of the PLQY of the PQDs, it is essential to diminish the non-radiative charge recombination processes. In this work, we approached two ways to control the non-radiative charge recombination processes through synthetic and post-synthetic processes. Firstly, we proposed how refinement of the conventional recrystallization process for PbI2 contributes to higher PLQY of the PQDs. Secondly, after halide exchange from CsPbI3 PQDs to CsPbBr3, through an in situ spectroelectrochemical setup, we monitored the positive correlation between bromide deposition of on the surface of the perovskite and photoluminescence improvement of the CsPbBr3 perovskite film through electrodeposition. These two strategies could provide a way to enhance the photophysical properties of the perovskites for application to various perovskite-based optoelectronic devices. [ABSTRACT FROM AUTHOR]

[Display omitted] • The detailed redox process of the perovskite quantum dots shown in the cyclic voltammograms was identified. • The irreversible electrochemical reaction products with their physical states of the perovskite quantum dots were tracked. • By tracking in-situ spectroelectrochemical condition, the effect of applied potential and the electrochemically reacted products from the perovskite quantum dots was identified. Multidimensional ABX 3 hybrid perovskites three-dimensionally confined dot-shaped structure demonstrate versatile potential to photoelectrochemical cells for water splitting, hydrogen generation, solar cells, and light-emitting diodes. To apply perovskite quantum dots (PQDs) to solar-driven chemistry and optoelectronic devices, understanding the photoinduced charge carrier dynamics of PQDs under electrochemical conditions or applied bias are important. In this study, the detailed transformation mechanism of formamidinium lead iodide perovskite quantum dots under electrochemical conditions was studied by tracking the products of the reaction through cyclic voltammetry, X-ray photoemission spectroscopy, in-situ UV–visible spectroelectrochemistry, etc. Through comprehensive characterizations, the mechanism of irreversible oxidative transformation of perovskite quantum dots was presented. This study provides deeper insight into the electrochemical behavior of PQDs for successful solar-driven chemistry and optoelectronic device applications. [ABSTRACT FROM AUTHOR]