Abstract
Promoters and precursors can control oxide phase, dispersion, and per-site reactivity of supported oxide catalysts. Previously, dispersed FeOxâSiO2 resulted from Fe3+ ethylenediaminetetraacetate (FeEDTAâ) precursors, with NaFeEDTA giving enhanced dispersion and oxidation rates vs. NH4FeEDTA. Here, catalysts were synthesized by sequential alkali deposition and Fe3+ impregnation. At up to 0.9Fenmâ2 from NH4FeEDTA and equimolar alkali, UVâvisible and H2 TPR were consistent with isolated Fe3+ and small FeOx clusters. Omitting alkali, using Fe(NO3)3, or using Fe/alkali >1 gave evidence of larger agglomerates. For Fe/alkali â€1 on non-porous SiO2, initial turnover frequencies in adamantane oxidation using H2O2 were independent of surface density. TOF increased as 6.3, 8.8, 15.4, and 20.9 (±0.3)ksâ1 for Li+, Na+, K+, and Cs+, respectively, increasingly linearly with decreasing electronegativity. These results give a synthesisâstructureâfunction taxonomy with alkali as an electronic and structural promoter of dispersed FeOx species for alkane selective oxidation.
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