Abstract
Ceria is a technologically important material with applications in catalysis, emissions control and solid-oxide fuel cells. Nanostructured ceria becomes profoundly more active due to its enhanced surface area to volume ratio, reactive surface oxygen vacancy concentration and superior oxygen storage capacity. Here we report the synthesis of nanostructured ceria using the green Deep Eutectic Solvent reline, which allows morphology and porosity control in one of the less energy-intensive routes reported to date. Using wide Q-range liquid-phase neutron diffraction, we elucidate the mechanism of reaction at a molecular scale at considerably milder conditions than the conventional hydrothermal synthetic routes. The reline solvent plays the role of a latent supramolecular catalyst where the increase in reaction rate from solvent-driven pre-organization of the reactants is most significant. This fundamental understanding of deep eutectic-solvothermal methodology will enable future developments in low-temperature synthesis of nanostructured ceria, facilitating its large-scale manufacturing using green, economic, non-toxic solvents.
Highlights
Ceria is a technologically important material with applications in catalysis, emissions control and solid-oxide fuel cells
We demonstrate that reline acts as a latent supramolecular catalyst by bringing the reactive components together in the presence of water, which at the same time acts as a directing agent
Reline and its aqueous mixtures are compatible with metal ions, including common ceria precursors such as Ce(NO3)[3] Á 6H2O or CeCl3, negating the need for the high concentration of solubilizing base that is required in equivalent hydrothermal synthesis
Summary
Ceria is a technologically important material with applications in catalysis, emissions control and solid-oxide fuel cells. The reline solvent plays the role of a latent supramolecular catalyst where the increase in reaction rate from solvent-driven pre-organization of the reactants is most significant This fundamental understanding of deep eutectic-solvothermal methodology will enable future developments in low-temperature synthesis of nanostructured ceria, facilitating its large-scale manufacturing using green, economic, non-toxic solvents. Solvothermal methods, reviewed by Walton[14], are a interesting development, as synthetic control is obtained by direct modification of the solvent environment In this context, Deep Eutectic Solvents (DESs) are an extended class of ionic liquids (ILs) made by complexing a (typically ammonium halide) salt with hydrogen bond donor molecules, depressing the glass transition temperature (Tg) at the eutectic molar ratio[15]. The solvent environment acts as an organic structuring framework, whereas the DES delivers templating agents from thermal degradation
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