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Compositional variation in hybrid organic-inorganic lead halide perovskites : kinetically- versus thermodynamically-controlled synthesis

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Tian_2021_CM_Compositional_AAM.pdf (1.557Mb)
Date
25/05/2021
Author
Tian, Jiyu
Zysman-Colman, Eli
Morrison, Finlay D.
Keywords
QD Chemistry
DAS
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Abstract
The formation and study of partial solid solutions in Az1-xFAxPbBr3, using reportedly similar sized cations azetidinium (Az+) and formamidinium (FA+), was explored via mechanosynthesis and precipitation synthesis. The composition and lattice parameters of samples from both syntheses were analyzed by 1H NMR and Rietveld refinement of powder X-ray diffraction. A clear mismatch in the composition of the perovskite was found between the precipitated samples and the corresponding solutions. Such a mismatch was not observed for samples obtained via mechanosynthesis. The discrepancy suggests products are kinetically-controlled during precipitation, compared to thermodynamically controlled mechanosynthesis. Furthermore, the cell volume as a function of composition in both hexagonal, 6H (Az-rich) and cubic, 3C (FA-rich) perovskite solid solutions suggests that FA+ is actually smaller than Az+, contradicting the literature. In the 3C (Az-poor) solid solutions, the extent of Az1-xFAxPbBr3 is unexpectedly smaller than in the corresponding methylammonium (MA+) system, Az1-xMAxPbBr3, which suggests that the extent of solid solution formation in these halide perovskites is predominantly dependent on the average A-cation size while the size mismatch plays a lesser role in comparison to oxides.
Citation
Tian , J , Zysman-Colman , E & Morrison , F D 2021 , ' Compositional variation in hybrid organic-inorganic lead halide perovskites : kinetically- versus thermodynamically-controlled synthesis ' , Chemistry of Materials , vol. 33 , no. 10 , pp. 3650-3659 . https://doi.org/10.1021/acs.chemmater.1c00470
Publication
Chemistry of Materials
Status
Peer reviewed
DOI
https://doi.org/10.1021/acs.chemmater.1c00470
ISSN
0897-4756
Type
Journal article
Rights
Copyright © 2021 American Chemical Society. This work has been made available online in accordance with publisher policies or with permission. Permission for further reuse of this content should be sought from the publisher or the rights holder. This is the author created accepted manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1021/acs.chemmater.1c00470
Description
Authors thank the Chinese Scholarship Council and the University of St Andrews for Ph.D. Studentship support (to JT, CSC No. 201603780020).
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  • University of St Andrews Research
URI
http://hdl.handle.net/10023/25361

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