Predictive design of engineered multifunctional solid catalysts

Abstract

The ability to devise and design multifunctional active sites at the nanoscale, by drawing on the intricate ability of enzymes to evolve single-sites with distinctive catalytic function, has prompted complimentary and concordant developments in the field of catalyst design and in situ operando spectroscopy. Innovations in design-application approach have led to a more fundamental understanding of the nature of the active site and its mechanistic influence at a molecular level, that have enabled robust structure-property correlations to be established, which has facilitated the dextrous manipulation and predictive design of redox and solid -acid sites for industrially-significant, sustainable catalytic transformations.

Influence of dopant substitution mechanism on catalytic properties within hierarchical architectures

“…The Al-O-P bonds in the AlPO architecture are more ionic in character than the bonds found within zeolites, and, hence, these materials are far more amenable to a wider range of isomorphous substitution than zeolites. AlPOs, indeed, have proved themselves to be extremely compositionally diverse with more than 20 different transition metals being substituted into the framework (in a tetrahedral geometry) with various oxidation states [19,20]. Hence, these frameworks have the potential to combine a specific coordination geometry, with isolated catalytically active sites, in order to create novel, robust, superior catalyst with high activities and selectivities.…”

Structure of the Catalytic Active Sites in Vanadium-Doped Aluminophosphate Microporous Materials. New Evidence from Spin Density Studies

“…5 Of particular importance for oxidation reactions are the so-called MeAPO materials in which Al ions are replaced by redox-active transition metals, such as Co, Mn, Fe, Cr etc. [6][7][8][9][10] These materials combine the reactivity of the redox-active cations with high surface area and the unique spatial constraints imposed by the molecular dimensions of their porous network.…”

Spectroscopic investigation into the design of solid–acid catalysts for the low temperature dehydration of ethanol

“…Zeotype materials have been implemented industrially for similar reactions. [8,9] The ability to confine active-sites within a microporous framework garners great control over the reactants accessing the active site, the intermediary species formed, and the products leaving the active site. Aluminophosphates (AlPOs) have analogous framework topologies as zeolites, though instead of being constructed from corner-sharing SiO 4 tetrahedra, AlPOs are formed from alternating AlO 4 and PO 4 tetrahedra connected by Al-O-P bonds.…”