In this work, we explore the synthesis of layered double hydroxide (LDH) particles containing different molar ratios of Gd3+ and Dy3+ cations. A single crystalline phase was obtained for Zn2.0Al0.75Gd0.125Dy0.125-LDH and Zn2.0Al0.5Gd0.25Dy0.25-LDH, and their efficiency as contrast agents was evaluated by T1- and T2-weighted magnetic resonance imaging (MRI). Both GdDy-LDHs exhibited longitudinal relaxivity (r1) higher than a commercial reference. The highest contrast in the T1 mode was achieved with the Zn2.0Al0.75Gd0.125Dy0.125-LDH, which contained the lowest concentration of lanthanides; this efficiency is related to the lowest amount of carbonate anions complexing the lanthanide sites. On the contrary, the best contrast in the T2 mode was achieved with Zn2.0Al0.5Gd0.25Dy0.25-LDH. Zn2.0Al0.75Gd0.125Dy0.125-LDH and Zn2.0Al0.5Gd0.25Dy0.25-LDH presented r2/r1 ratios of 7.9 and 22.5, respectively, indicating that the inclusion of gadolinium and dysprosium into layered structures is a promising approach to the development of efficient bimodal (T1/T2) MRI contrast agents.
Zinc/aluminum layered double hydroxide (LDH) particles were prepared by alkaline precipitation in the presence of dysprosium and dysprosium/gadolinium cations. The particles formed were stable against exchange reactions with folate or glucuronate ions since these organic ions exclusively functionalized the external surface of the layered double hydroxides. While the dysprosium derivatives reached magnetization susceptibilities between 2.06 Â 10 À5 and 2.20 Â 10 À5 cm 3 /g, the samples simultaneously containing dysprosium and gadolinium decreased to a range between 1.08 Â 10 À5 and 1.73 Â 10 À5 cm 3 /g. This last sample was tested as a magnetic resonance imaging contrast agent and demonstrated a reduction in T1 and T2 relaxation times in a linear dependence with the LDH concentration. The oxidative stress assays in rat liver mitochondria demonstrated the low toxicity of the composition simultaneously containing dysprosium and gadolinium as well as the functionalization product with glucuronate ions, suggesting the potential of these particles to design alternative MRI contrast agents.
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