Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.322
Publication date: 18th December 2023
Metal halide perovskites (MHPs) are extremely appealing emerging materials for photocatalytically active heterojunctions, thanks to their ability to promote light-driven reactions. However, a comprehensive understanding of photoexcitation and charge transfer mechanisms, as well as predictive models for photocatalytic performances are still missing. We present here a robust method to investigate photocatalytic activity of MHP heterojunctions in a variety of reactions, that combines in synergy a wide array of experimental techniques with advanced computational modelling. For all the studied compounds, we were able to assess a clear link between the photocatalytic activity and optoelectronic properties of the materials, in particular by exploiting ultrafast spectroscopy techniques to study available transitions and carrier dynamics as a function of the perovskite loading and finding a connection with the performance of the material.
More in detail, we studied heterojunctions obtained by combining graphitic carbon nitride (g-C3N4) with different kinds of lead-free perovskites to enhance selected features. We focused first on double perovskite Cs3Bi2Br9, where hydrogen photogeneration rate was successfully controlled by tuning the perovskite loading in the Cs3Bi2Br9/g-C3N4 mixture.[1] We also studied Ge-based layered 2D perovskite and g-C3N4 for light-induced hydrogen evolution: we showed how, thanks to organic cation engineering, perovskites based on 4-phenylbenzilammonium (PhBz), such as PhBz2GeBr4 and PhBz2GeI4, result in hydrogen production with promising air and water stability.[2] Recently, we have extended our study to a double perovskite mixture, namely Cs2AgBiCl6/g-C3N4, used both for solar-driven hydrogen generation and nitrogen reduction, with an activity strongly depending on the perovskite loading.[3] Through advanced spectroscopic investigation and density function theory (DFT) modelling we have identified the perovskite loading that allows the best performance of the heterojunction and, most importantly, accounted for the microscopic processes responsible for the photocatalytic performance. Our results are showing a systematic approach of MHP-based heterojunctions that is of crucial importance to get the ability to engineer and optimize novel materials for photocatalysis.
L.M., A.S., A.P. acknowledge support from the Ministero dell’Università e della Ricerca (MUR) and the University of Pavia through the program “Dipartimenti di Eccellenza 2023–2027. L.M., E.M. and A.L. acknowledge support from the Ministero dell’Università e della Ricerca (MUR) through PRIN Project REVOLUTION (2022HRZH7P). A. P. acknowledges
support from the Ministero dell’Università e della Ricerca (MUR) through PRIN Project PHOTOFIX (2022TWKM4X). E.M. and S.C. acknowledge project Ricerca@Cnr PHOTOCAT (CUP B93C21000060006). F.D.A. acknowledges funds by the European Union - NextGenerationEU under the Italian Ministry of University and Research (MUR) National Innovation Ecosystem grant ECS00000041 - VITALITY. S.C. acknowledges support from the Ministero dell’Università e della Ricerca (MUR) through PRIN Project INTERFACE (2022HWWW3S). L.M. and C.T. acknowledge financial support from R.S.E. SpA (Ricerca sul Sistema Energetico).
A.S. acknowledges funding from PON AIM1809115 Num. Attività 2, Linea 2.1.
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