Catalytic materials based on silica and alumina: Structural features and generation of surface acidity

Silica-alumina catalytic materials: A critical review

One‐Step Selective Hydroxylation of Benzene to Phenol

Photocatalytic hydroxylation of benzene to phenol was achieved by using O2 as an oxidant as well as an oxygen source with a cyano-bridged polynuclear metal complex containing FeII and RuII incorporated in mesoporous silica–alumina ([Fe(H2O)3]2[Ru(CN)6]@sAl-MCM-41). An apparent turnover number (TON) of phenol production per the monomer unit of [Fe(H2O)3]2[Ru(CN)6] was 41 for 59 h. The cyano-bridged polynuclear metal complex, [Fe(H2O)3]2[Ru(CN)6], exhibited catalytic activity for thermal hydroxylation of benzene by H2O2 in acetonitrile (MeCN), where the apparent TON of phenol production reached 393 for 60 h. The apparent TON increased to 2500 for 114 h by incorporating [Fe(H2O)3]2[Ru(CN)6] in sAl-MCM-41. Additionally, [Fe(H2O)3]2[Ru(CN)6] acts as a water oxidation catalyst by using [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) and Na2S2O8 as a photosensitizer and a sacrificial electron acceptor as evidenced by 18O-isotope labeling experiments. Photoirradiation of an O2-saturated MeCN solution containing [Fe(H2O)3]2[...

/pdf/photocatalytic-hydroxylation-of-benzene-by-dioxygen-to-2zm9w5g2c1.pdf

Photocatalytic Hydroxylation of Benzene by Dioxygen to Phenol with a Cyano-Bridged Complex Containing Fe(II) and Ru(II) Incorporated in Mesoporous Silica-Alumina.

In the homogenous phase, redox catalysts are often deactivated by bimolecular reactions. For example, the charge‐separated state of photoredox catalysts decayed via bimolecular back electron transfer reactions between the charge‐separated molecules to decrease the lifetimes of the catalytically active species. When photoredox catalysts are immobilized on solid supports, the lifetime of the charge‐separated state was remarkably elongated to enhance the photocatalytic activity. Immobilization of photoredox catalysts on electrodes is required for photocurrent generation, leading to development of solar cells. Metal‐oxygen intermediates, which are active for oxidation of various substrates including water oxidation, are also deactivated via bimolecular reactions to produce inactive forms such as dinuclear metal bis‐μ‐oxo complexes. Immobilization of metal complex catalysts on solid supports prohibits the bimolecular deactivation, enhancing the catalytic activity and stability. This Review focuses on recent development of immobilization of both organic and inorganic molecular catalysts on various supports for enhancement of the catalytic activity, selectivity and stability in thermal and photoinduced redox reactions.

Immobilization of Molecular Catalysts for Enhanced Redox Catalysis

Aluminum in mesoporous silica–alumina

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Aluminum in mesoporous silica–alumina