| Title: |
Persistent nucleation and size dependent attachment kinetics produce monodisperse PbS nanocrystals |
| Authors: |
Abécassis, Benjamin; Greenberg, Matthew; Bal, Vivekananda; Mcmurtry, Brandon; Campos, Michael; Guillemeney, Lilian; Mahler, Benoit; Prevost, Sylvain; Sharpnack, Lewis; Hendricks, Mark; Derosha, Daniel; Bennett, Ellie; Saenz, Natalie; Peters, Baron; Owen, Jonathan |
| Contributors: |
Laboratoire de Chimie - UMR5182 (LC); École normale supérieure de Lyon (ENS de Lyon); Université de Lyon-Université de Lyon-Université Claude Bernard Lyon 1 (UCBL); Université de Lyon-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS); Columbia University New York; University of Illinois at Urbana-Champaign Urbana (UIUC); University of Illinois System; iLM - Luminescence (iLM - LUMINESCENCE); Institut Lumière Matière Villeurbanne (ILM); Université Claude Bernard Lyon 1 (UCBL); Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL); Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS); Institut Laue-Langevin (ILL); University of California Santa Barbara (UC Santa Barbara); University of California (UC); Whitman College |
| Source: |
ISSN: 2041-6520. |
| Publisher Information: |
CCSD; The Royal Society of Chemistry |
| Publication Year: |
2022 |
| Collection: |
HAL Lyon 1 (University Claude Bernard Lyon 1) |
| Subject Terms: |
[SPI]Engineering Sciences [physics]; [CHIM]Chemical Sciences; [PHYS]Physics [physics] |
| Description: |
International audience ; Modern syntheses of colloidal nanocrystals yield extraordinarily narrow size distributions that are believed toresult from a rapid “burst of nucleation” (La Mer, JACS, 1950, 72(11), 4847–4854) followed by diffusionlimited growth and size distribution focusing (Reiss, J. Chem. Phys., 1951, 19, 482). Using a combinationof in situ X-ray scattering, optical absorption, and 13C nuclear magnetic resonance (NMR) spectroscopy,we monitor the kinetics of PbS solute generation, nucleation, and crystal growth from three thioureaprecursors whose conversion reactivity spans a 2-fold range. In all three cases, nucleation is found to beslow and continues during >50% of the precipitation. A population balance model based on a sizedependent growth law (1/r) fits the data with a single growth rate constant (kG) across all threeprecursors. However, the magnitude of the kG and the lack of solvent viscosity dependence indicatesthat the rate limiting step is not diffusion from solution to the nanoparticle surface. Several surfacereaction limited mechanisms and a ligand penetration model that fits data our experiments using a singlefit parameter are proposed to explain the results |
| Document Type: |
article in journal/newspaper |
| Language: |
English |
| DOI: |
10.1039/D1SC06134H |
| Availability: |
https://hal.science/hal-03652747; https://hal.science/hal-03652747v1/document; https://hal.science/hal-03652747v1/file/d1sc06134h.pdf; https://doi.org/10.1039/D1SC06134H |
| Rights: |
https://creativecommons.org/licenses/by-nc/4.0/ ; info:eu-repo/semantics/OpenAccess |
| Accession Number: |
edsbas.ABD57EB3 |
| Database: |
BASE |