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Carboxylic-acid-passivated metal oxide nanocrystals : ligand exchange characteristics of a new binding motif

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Abstract
Ligand exchange is central in the processing of inorganic nanocrystals (NCs) and requires understanding of surface chemistry. Studying sterically stabilized HfO2 and ZrO2 NCs using H-1 solution NMR and IR spectroscopy as well as elemental analysis, this paper demonstrates the reversible exchange of initial oleic acid ligands for octylamine and self-adsorption of oleic acid at NC surfaces. Both processes are incompatible with an X-type binding motif of carboxylic acids as reported for sulfide and selenide NCs. We argue that this behavior stems from the dissociative adsorption of carboxylic acids at the oxide surface. Both proton and carboxylate moieties must be regarded as X-type ligands yielding a combined X-2 binding motif that allows for self-adsorption and exchange for L-type ligands.
Keywords
ligand exchange, CdSe, nanoparticles, NMR spectroscopy, surface chemistry, CDSE QUANTUM DOTS, SURFACE-CHEMISTRY, COLLOIDAL NANOCRYSTALS, NANOPARTICLES

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Citation

Please use this url to cite or link to this publication:

Chicago
De Roo, Jonathan, Yolanda Justo Zarraquiños, Katrien De Keukeleere, Freya Van den Broeck, José Martins, Isabel Van Driessche, and Zeger Hens. 2015. “Carboxylic-acid-passivated Metal Oxide Nanocrystals : Ligand Exchange Characteristics of a New Binding Motif.” Angewandte Chemie-international Edition 54 (22): 6488–6491.
APA
De Roo, J., Justo Zarraquiños, Y., De Keukeleere, K., Van den Broeck, F., Martins, J., Van Driessche, I., & Hens, Z. (2015). Carboxylic-acid-passivated metal oxide nanocrystals : ligand exchange characteristics of a new binding motif. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 54(22), 6488–6491.
Vancouver
1.
De Roo J, Justo Zarraquiños Y, De Keukeleere K, Van den Broeck F, Martins J, Van Driessche I, et al. Carboxylic-acid-passivated metal oxide nanocrystals : ligand exchange characteristics of a new binding motif. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION. 2015;54(22):6488–91.
MLA
De Roo, Jonathan, Yolanda Justo Zarraquiños, Katrien De Keukeleere, et al. “Carboxylic-acid-passivated Metal Oxide Nanocrystals : Ligand Exchange Characteristics of a New Binding Motif.” ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 54.22 (2015): 6488–6491. Print.
@article{6842958,
  abstract     = {Ligand exchange is central in the processing of inorganic nanocrystals (NCs) and requires understanding of surface chemistry. Studying sterically stabilized HfO2 and ZrO2 NCs using H-1 solution NMR and IR spectroscopy as well as elemental analysis, this paper demonstrates the reversible exchange of initial oleic acid ligands for octylamine and self-adsorption of oleic acid at NC surfaces. Both processes are incompatible with an X-type binding motif of carboxylic acids as reported for sulfide and selenide NCs. We argue that this behavior stems from the dissociative adsorption of carboxylic acids at the oxide surface. Both proton and carboxylate moieties must be regarded as X-type ligands yielding a combined X-2 binding motif that allows for self-adsorption and exchange for L-type ligands.},
  author       = {De Roo, Jonathan and Justo Zarraqui{\~n}os, Yolanda and De Keukeleere, Katrien and Van den Broeck, Freya and Martins, Jos{\'e} and Van Driessche, Isabel and Hens, Zeger},
  issn         = {1433-7851},
  journal      = {ANGEWANDTE CHEMIE-INTERNATIONAL EDITION},
  keyword      = {ligand exchange,CdSe,nanoparticles,NMR spectroscopy,surface chemistry,CDSE QUANTUM DOTS,SURFACE-CHEMISTRY,COLLOIDAL NANOCRYSTALS,NANOPARTICLES},
  language     = {eng},
  number       = {22},
  pages        = {6488--6491},
  title        = {Carboxylic-acid-passivated metal oxide nanocrystals : ligand exchange characteristics of a new binding motif},
  url          = {http://dx.doi.org/10.1002/anie.201500965},
  volume       = {54},
  year         = {2015},
}

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