Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
DOI: https://doi.org/10.29363/nanoge.matsusfall.2024.158
Publication date: 28th August 2024
The request for sustainable and renewable energy sources has motivated a significant shift toward innovative methods for producing and storing clean energy through green solar fuels. Photocatalytically active heterojunctions based on metal halide perovskites (MHPs) are drawing important interest for their tuneable ability to promote several redox reactions. This study investigates two composite systems: a classic double perovskite-based, Cs2AgBiCl6/g-C3N4,1 and a vacancy-ordered perovskite-based, Cs2SnBr6/g-C3N4. The first system has been studied and employed for both solar-driven hydrogen generation from chloride media and nitrogen reduction and the second one for nitrogen reduction. The efficiency of the Cs2AgBiCl6/g-C3N4 system depends on the relative amounts of perovskite and carbon nitride to promote the two reactions. Spectroscopic investigations and density functional theory (DFT) modelling reveal that perovskite halide vacancies are primary reactive sites for hydrogen generation and can be, together with g-C3N4 nitrogen vacancies crucial also for nitrogen reduction.1 On these bases, again through a combined experimental and computational approach, we provide a detailed framework of the mechanism supporting the efficient nitrogen reduction reaction to ammonia observed in Cs2SnBr6/g-C3N4 system. The vacancy-ordered perovskite is characterized by a higher surface density of halide vacancies than the double perovskite and then the Cs2SnBr6/g-C3N4 system achieves the highest ammonia evolution rate of 266 μmol g-1 h-1. Photoluminescence studies and differential transmission measurements stress the importance of compositional engineering in enhancing photocatalysis efficiency for both reactions. This work represents a significant advancement in photocatalytic green fuels production, especially in the field of nitrogen photofixation, proposing materials and structures that can potentially improve sustainable ammonia production, thereby contributing to energy independence and reduced carbon emissions.
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).
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