The Reactivity of CsPbBr3Nanocrystals toward Acid/Base Ligands

Autor: Francesco Zaccaria, Baowei Zhang, Luca Goldoni, Muhammad Imran, Juliette Zito, Bas van Beek, Simone Lauciello, Luca De Trizio, Liberato Manna, Ivan Infante
Přispěvatelé: Theoretical Chemistry, AIMMS
Jazyk: angličtina
Rok vydání: 2022
Předmět:
Zdroj: ACS Nano, 16(1), 1444-1455. American Chemical Society
Zaccaria, F, Zhang, B, Goldoni, L, Imran, M, Zito, J, van Beek, B, Lauciello, S, De Trizio, L, Manna, L & Infante, I 2022, ' The Reactivity of CsPbBr 3 Nanocrystals toward Acid/Base Ligands ', ACS Nano, vol. 16, no. 1, pp. 1444-1455 . https://doi.org/10.1021/acsnano.1c09603
ISSN: 1936-0851
DOI: 10.1021/acsnano.1c09603
Popis: The interaction of lead bromide perovskite nanocrystals with charged ligands, such as salts, zwitterions, or acid-base pairs, has been extensively documented over the past few years. On the other hand, little is known about the reactivity of perovskite nanocrystals toward neutral ligands. To fill this gap, in this work we study the interaction of CsPbBr3 nanocrystals passivated with didodecyldimethylammonium bromide (DDABr) toward a series of exogenous acid/base ligands using a combined computational and experimental approach. Our analysis indicates that DDABr-capped nanocrystals are inert toward most ligands, except for carboxylic, phosphonic, and sulfonic acids. In agreement with the calculations, our experimental results indicate that the higher the acidity of the ligands employed in the treatment, the more etching is observed. In detail, dodecylbenzenesulfonic acid (pKa = -1.8) is found to etch the nanocrystals, causing their complete degradation. On the other hand, oleic and oleylphosphonic acids (pKa 9.9 and 2, respectively) interact with surface-bound DDA molecules, causing their displacement as DDABr in various amounts, which can be as high as 40% (achieved with oleylphosphonic acid). Despite the stripping of DDA ligands, the optical properties of the nanocrystals, as well as structure and morphology, remain substantially unaffected, empirically demonstrating the defect tolerance characterizing such materials. Our study provides not only a clear overview on the interaction between perovskite nanocrystals and neutral ligands but also presents an effective ligand stripping strategy.
Databáze: OpenAIRE