Samenvatting
Bandgap-tuneable mixed-halide 3D perovskites are of interest for multi-junction solar cells, but suffer from photoinduced spatial halide segregation. Mixed-halide 2D perovskites are more resistant to halide segregation and are promising coatings for 3D perovskite solar cells. The properties of mixed-halide compositions depend on the local halide distribution, which is challenging to study at the level of single octahedra. In particular, it has been suggested that there is a preference for occupation of the distinct axial and equatorial halide sites in mixed-halide 2D perovskites. 207Pb NMR can be used to probe the atomic-scale structure of lead-halide materials, but although the isotropic 207Pb shift is sensitive to halide stoichiometry, it cannot distinguish configurational isomers. Here, we use 2D isotropic–anisotropic correlation 207Pb NMR and relativistic DFT calculations to distinguish the [PbX6] configurations in mixed iodide–bromide 3D FAPb(Br1−xIx)3 perovskites and 2D BA2Pb(Br1−xIx)4 perovskites based on formamidinium (FA+) and butylammonium (BA+), respectively. We find that iodide preferentially occupies the axial site in BA-based 2D perovskites, which may explain the suppressed halide mobility.
Originele taal-2 | Engels |
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Artikelnummer | e202314856 |
Aantal pagina's | 10 |
Tijdschrift | Angewandte Chemie - International Edition |
Volume | 63 |
Nummer van het tijdschrift | 13 |
Vroegere onlinedatum | 2 feb. 2024 |
DOI's | |
Status | Gepubliceerd - 22 mrt. 2024 |
Bibliografische nota
Publisher Copyright:© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
Financiering
This work was supported by SNSF grant number 200020_212046. M.A.H. acknowledges a H2020 Marie Sk\u0142odowska-Curie Individual fellowship with grant number 101024144. We would like to thank Prof. Grandinetti, Dr. Srivastava, and Mr. Giammar (Ohio State University) for support and advice in using Mrsimulator. Open Access funding provided by \u00C9cole Polytechnique F\u00E9d\u00E9rale de Lausanne. This work was supported by SNSF grant number 200020_212046. M.A.H. acknowledges a H2020 Marie Sk\u0142odowska\u2010Curie Individual fellowship with grant number 101024144. We would like to thank Prof. Grandinetti, Dr. Srivastava, and Mr. Giammar (Ohio State University) for support and advice in using Mrsimulator. Open Access funding provided by \u00C9cole Polytechnique F\u00E9d\u00E9rale de Lausanne.
Financiers | Financiernummer |
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H2020 Marie Skłodowska-Curie Actions | 101024144 |
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung | 200020_212046 |
Vingerafdruk
Duik in de onderzoeksthema's van 'Axial–Equatorial Halide Ordering in Layered Hybrid Perovskites from Isotropic–Anisotropic 207Pb NMR'. Samen vormen ze een unieke vingerafdruk.Datasets
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Data for Axial–Equatorial Halide Ordering in Layered Hybrid Perovskites from Isotropic–Anisotropic 207Pb NMR
Hope, M. A. (Ontwerper), Cordova, M. (Ontwerper), Mishra, A. (Ontwerper), Gunes, U. (Ontwerper), Caiazzo, A. (Ontwerper), Datta, K. (Ontwerper), Janssen, R. (Ontwerper) & Emsley, L. (Ontwerper), Zenodo, 5 feb. 2024
DOI: 10.5281/zenodo.8324046, https://zenodo.org/records/8324046
Dataset