Published February 23, 2022 | Version v1
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Colloidal-ALD Grown Hybrid Shells Nucleate via a Ligand–Precursor Complex

  • 1. Laboratory of Nanochemistry for Energy (LNCE), Institute of Chemical Sciences and Engineering (ISIC), École Polytechnique Fédérale de Lausanne, CH-1950 Sion, Switzerland
  • 2. Laboratory of Magnetic Resonance (LMR), Institute of Chemical Sciences and Engineering (ISIC), École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland

Description

Colloidal atomic layer deposition (c-ALD) enables the growth of hybrid organic–inorganic oxide shells with tunable thickness
at the nanometer scale around ligand-functionalized inorganic nanoparticles (NPs). This recently developed method has demonstrated improved stability of NPs and of their dispersions, a key requirement for their application.
Nevertheless, the mechanism by which the inorganic shells form is still unknown, as is the nature of multiple complex interfaces between the NPs, the organic ligands functionalizing the surface, and the shell. Here, we demonstrate that carboxylate ligands are the key element that enables the synthesis of these core–shell structures. Dynamic nuclear polarization surface-enhanced nuclear magnetic resonance spectroscopy (DNP SENS) in combination with density functional theory (DFT) structure calculations shows that the addition of the aluminum organometallic precursor forms a ligand–precursor complex that interacts with the NP surface. This ligand–precursor complex is the first step for the nucleation of the shell and enables its further growth.

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Additional details

Related works

Is supplemented by
Journal article: 10.1021/jacs.1c12538 (DOI)

Funding

NCCR Catalysis (phase I) 51NF40_180544
Swiss National Science Foundation