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Utilizing self-exchange to address the binding of carboxylic acid ligands to CdSe quantum dots

Bernd Fritzinger UGent, Richard Capek UGent, Karel Lambert UGent, José Martins UGent and Zeger Hens UGent (2010) JOURNAL OF THE AMERICAN CHEMICAL SOCIETY. 132(29). p.10195-10201
abstract
We use solution NMR techniques to analyze the organic/inorganic interface of CdSe quantum dots (Q-CdSe) synthesized using oleic acid as a surfactant. It is shown that the resulting Q-CdSe are stabilized by tightly bound oleic acid species that only exchange upon addition of free oleic acid. The NMR analysis points toward a two-step exchange mechanism where free ligands are initially physisorbed within the ligand shell to end up as bound, chemisorbed ligands in a second step. Importantly, we find that every ligand is involved in this exchange process. By addition of oleic acid with a deuterated carboxyl headgroup, we demonstrate that the bound ligands are oleate ions and not oleic acid molecules. This explains why a dynamic adsorption/desorption equilibrium only occurs in the presence of excess free oleic acid, which donates the required proton. Comparing the number of oleate ligands to the excess cadmium per CdSe quantum dot, we find a ratio of 2:1. This completes the picture of Q-CdSe as organic/inorganic entities where the surface excess of Cd2+ is balanced by a double amount of oleate ligands, yielding overall neutral nanoparticles.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
COLLOIDAL NANOCRYSTALS, SURFACE STOICHIOMETRY, SEMICONDUCTOR NANOCRYSTALS, FIELD GRADIENT NMR, PBSE NANOCRYSTAL SOLIDS, ELECTRICAL-PROPERTIES, SOLAR-CELLS, NANOPARTICLES, SPECTROSCOPY, GROWTH
journal title
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
J. Am. Chem. Soc.
volume
132
issue
29
pages
10195 - 10201
Web of Science type
Article
Web of Science id
000280227700056
JCR category
CHEMISTRY, MULTIDISCIPLINARY
JCR impact factor
9.019 (2010)
JCR rank
11/142 (2010)
JCR quartile
1 (2010)
ISSN
0002-7863
DOI
10.1021/ja104351q
language
English
UGent publication?
yes
classification
A1
copyright statement
I have transferred the copyright for this publication to the publisher
id
1044641
handle
http://hdl.handle.net/1854/LU-1044641
date created
2010-09-22 13:58:04
date last changed
2010-09-23 08:38:42
@article{1044641,
  abstract     = {We use solution NMR techniques to analyze the organic/inorganic interface of CdSe quantum dots (Q-CdSe) synthesized using oleic acid as a surfactant. It is shown that the resulting Q-CdSe are stabilized by tightly bound oleic acid species that only exchange upon addition of free oleic acid. The NMR analysis points toward a two-step exchange mechanism where free ligands are initially physisorbed within the ligand shell to end up as bound, chemisorbed ligands in a second step. Importantly, we find that every ligand is involved in this exchange process. By addition of oleic acid with a deuterated carboxyl headgroup, we demonstrate that the bound ligands are oleate ions and not oleic acid molecules. This explains why a dynamic adsorption/desorption equilibrium only occurs in the presence of excess free oleic acid, which donates the required proton. Comparing the number of oleate ligands to the excess cadmium per CdSe quantum dot, we find a ratio of 2:1. This completes the picture of Q-CdSe as organic/inorganic entities where the surface excess of Cd2+ is balanced by a double amount of oleate ligands, yielding overall neutral nanoparticles.},
  author       = {Fritzinger, Bernd and Capek, Richard and Lambert, Karel and Martins, Jos{\'e} and Hens, Zeger},
  issn         = {0002-7863},
  journal      = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY},
  keyword      = {COLLOIDAL NANOCRYSTALS,SURFACE STOICHIOMETRY,SEMICONDUCTOR NANOCRYSTALS,FIELD GRADIENT NMR,PBSE NANOCRYSTAL SOLIDS,ELECTRICAL-PROPERTIES,SOLAR-CELLS,NANOPARTICLES,SPECTROSCOPY,GROWTH},
  language     = {eng},
  number       = {29},
  pages        = {10195--10201},
  title        = {Utilizing self-exchange to address the binding of carboxylic acid ligands to CdSe quantum dots},
  url          = {http://dx.doi.org/10.1021/ja104351q},
  volume       = {132},
  year         = {2010},
}

Chicago
Fritzinger, Bernd, Richard Capek, Karel Lambert, José Martins, and Zeger Hens. 2010. “Utilizing Self-exchange to Address the Binding of Carboxylic Acid Ligands to CdSe Quantum Dots.” Journal of the American Chemical Society 132 (29): 10195–10201.
APA
Fritzinger, B., Capek, R., Lambert, K., Martins, J., & Hens, Z. (2010). Utilizing self-exchange to address the binding of carboxylic acid ligands to CdSe quantum dots. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 132(29), 10195–10201.
Vancouver
1.
Fritzinger B, Capek R, Lambert K, Martins J, Hens Z. Utilizing self-exchange to address the binding of carboxylic acid ligands to CdSe quantum dots. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY. 2010;132(29):10195–201.
MLA
Fritzinger, Bernd, Richard Capek, Karel Lambert, et al. “Utilizing Self-exchange to Address the Binding of Carboxylic Acid Ligands to CdSe Quantum Dots.” JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 132.29 (2010): 10195–10201. Print.