4.8 Article

The H-D-isotope effect of heavy water affecting ligand-mediated nanoparticle formation in SANS and NMR experiments

Journal

NANOSCALE
Volume 15, Issue 40, Pages 16413-16424

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d3nr02419a

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This study investigates the impact of heavy water (D2O) on CdS nanoparticle formation and colloidal stability. The results suggest that the isotopic effect of D2O influences nanoparticle formation by altering the equilibria and dynamics of ethylenediaminetetraacetate (EDTA) clusters in solution. Despite the stabilizing effect of EDTA in normal water, the colloidal stability of CdS nanoparticles is significantly reduced in heavy water.
An isotopic effect of normal (H2O) vs. heavy water (D2O) is well known to fundamentally affect the structure and chemical properties of proteins, for instance. Here, we correlate the results from small angle X-ray and neutron scattering (SAXS, SANS) with high-resolution scanning transmission electron microscopy to track the evolution of CdS nanoparticle size and crystallinity from aqueous solution in the presence of the organic ligand ethylenediaminetetraacetate (EDTA) at room temperature in both H2O and D2O. We provide evidence via SANS experiments that exchanging H2O with D2O impacts nanoparticle formation by changing the equilibria and dynamics of EDTA clusters in solution as investigated by nuclear magnetic resonance analysis. The colloidal stability of the CdS nanoparticles, covered by a layer of [Cd(EDTA)]2- complexes, is significantly reduced in D2O despite the strong stabilizing effect of EDTA in suspensions of normal water. Hence, conclusions about nanoparticle formation mechanisms from D2O solutions reveal limited transferability to reactions in normal water due to isotopic effects, which thus need to be discussed for contrast match experiments. Changing from H2O to D2O in CdS nanoparticle formation creates an isotopic effect impacting particle formation. SANS and NMR reveal different complex building constants with the EDTA ligand and how these affect colloidal stability too.

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