Preparation of Al/Fe-PILC clay catalysts from concentrated precursors: enhanced hydrolysis of pillaring metals and intercalation.

ABSTRACT: The modification of bentonite with Al-Fe species from different concentrated precursors at both stages: (i) the preparation of the (Al/Fe)-mixed pillaring solution and (ii) intercalation itself, was studied at lab scale. The final solids were characterized by X-ray fluorescence (XRF), X-ray diffraction (XRD), Cationic Exchange Capacity (CEC), textural analyses by nitrogen adsorption-desorption at 77 K, and hydrogen-temperature programmed reduction (H₂-TPR). Finally, the modified clays were assessed as active materials in the Catalytic Wet Peroxide Oxidation (CWPO) of phenol under very mild conditions through 1.0 h of reaction: T = 25.0 °C ± 0.1 °C, pH = 3.7, ambient pressure (76 kPa), and 0.5 g catalyst per dm³. Metal hydrolysis by the dissolution of elemental aluminium (final Total Metal Concentration TMC = 4.62 mol dm^-3) achieved the best results, decreasing the volume of solution per mass unit of clay required to successfully expand the layered starting mineral by a factor of close to 75, in comparison with the widespread conventional preparation using highly diluted Al-based pillaring solutions. Even in the absence of any solvent for the clay dispersion, the intercalating/pillaring method was shown to be favourable, as a novel strategy promoting the process intensification and subsequent preparation of Al/Fe- and other Al-based pillared clays at larger scales. The best catalyst prepared from concentrated precursors exhibited 79.1% phenol conversion, 19.3% TOC mineralization, and pretty low iron leaching (0.037 mg Fe dm^-3; ∼0.12% w/w) in such a short catalytic assessment; all these results were quite comparable or even exceeded those exhibited by the catalyst prepared from dilute precursors.

SUBMITTER: Vallejo CA 

PROVIDER: S-EPMC9057571 | biostudies-literature | 2020 Nov

REPOSITORIES: biostudies-literature