A novel synthesis route driving redox-precipitation reactions among MnVII, CeIII, and MnII precursors
in basic aqueous solution yields MnCeO
x
catalysts (Mnat/Ceat, 0.33−2.0) with a (quasi)molecular dispersion
of the active phase and enhanced textural properties in comparison to the conventional coprecipitation
method. The basic characteristics of the redox-precipitation process leading to a solid architecture missing
a substantial “long-range” crystalline order are discussed. With an excellent reproducibility and irrespective
of the Mnat/Ceat ratio, the redox-precipitation method also ensures unchanged textural, structural, and
chemical properties of the MnCeO
x
catalysts. As a much improved dispersion of the active phase, the
redox-precipitation route greatly promotes the redox behavior and the surface affinity toward gas-phase
oxygen of the MnCeO
x
system.
The effects of chemical composition, calcination temperature, and the addition of potassium on the physicochemical properties and reactivity of MnCeO x systems in the catalytic wet oxidation (CWO) of phenol with oxygen (T R ) 373 K; P R ) 1.0 MPa; w cat /w phenol ) 5) have been addressed. Characterization data of "fresh" and "spent" catalysts signal the occurrence of a typically heterogeneous reaction path, the surface reaction between the adsorbed intermediate(s), and activated oxygen species being the rate-determining step (rds). Basic relationships among structural properties, the redox pattern, and CWO activity provide evidence of the main catalyst design requirements. A new synthesis route based on the redox-precipitation reactions of various Mn and Ce precursors then yields MnCeO x catalysts with improved physicochemical features and superior CWO activity, in comparison to conventional coprecipitated systems.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.