Anthony K. Uriarte

Generation of active oxygen species on solid surfaces. Opportunity for novel oxidation technologies over zeolites

Generation of surface oxygen species and their role in partial oxidation reactions catalyzed by metal oxides are discussed. Main attention is paid to a new concept related to a recent discovery of remarkable ability of Fe complexes stabilized in a ZSM-5 matrix to generate a new form of surface oxygen (α-oxygen) from N2O. At room temperature, α-oxygen exhibits a high reactivity typical for the active oxygen of monooxygenases, and mimics its unique ability to perform selective oxidation of hydrocarbons. This opens new opportunity for creating novel technologies based on biomimetic strategy. A process of direct oxidation of benzene to phenol, recently demonstrated by Solutia on a pilot plant scale, is evidence of great potential of this approach.

Preparation and catalytic study of metal modified TS-1 in the oxidation of benzene to phenol by N2O

The titanosilicalite TS-1 samples modified by Al, V, Cr, Fe, Co and Ru were synthesized, characterized and tested in the title reaction. As with the earlier studied zeolite systems, Fe introduction into the TS-1 matrix produces α-sites that can catalyze the oxidation of benzene to phenol with high activity and selectivity. Other metals are shown to be inert. The quantitative dependencies of the catalytic activity on Fe content and on α-site concentration are discussed.

Nitrous oxide (N2O)—Waste to value

Waste N2O from adipic acid process is used a feedstock for novel single-step technology of manufacturing phenol from benzene (AlphOx process). The AlphOx process is discussed both as an integral part and key step of the new adipic acid manufacturing concept and as a stand-alone technology. Major developments in N2O recovery and purification from the adipic process waste stream, as well as in N2O on purpose manufacturing are presented.