Stable and Active Oxidation Catalysis by Cooperative Lattice Oxygen Redox on SmMn2O5 Mullite Surface.

The correlation between lattice oxygen (O) binding energy and O oxidation activity imposes a fundamental limit in developing oxide catalysts, simultaneously meeting the stringent thermal stability and catalytic activity standards for complete oxidation reactions under harsh conditions. Typically, strong O binding indicates a stable surface structure, but low O oxidation activity, and vice versa. Using nitric oxide (NO) catalytic oxidation as a model reaction, we demonstrate that this conflicting correlation can be avoided by cooperative lattice oxygen redox on SmMn2O5 mullite oxides, leading to stable and active oxide surface structures. The strongly bound neighboring lattice oxygen pair cooperates in NO oxidation to form bridging nitrate (NO3-) intermediates, which can facilely transform into monodentate NO3- by a concerted rotation with simultaneous O2 adsorption onto the resulting oxygen vacancy. Subsequently, monodentate NO3- species decompose to NO2 to restore one of the lattice oxygen atoms that act as a reversible redox center, and the vacancy can easily activate O2 to replenish the consumed one. This discovery not only provides insights into the cooperative reaction mechanism but also aids the design of oxidation catalysts with the strong O binding region, offering strong activation of O2, high O activity, and high thermal stability in harsh conditions.

Optimization of operating parameters for efficient photocatalytic inactivation of Escherichia coli based on a statistical design of experiments.

In this work, the individual and interaction effects of three key operating parameters of the photocatalytic disinfection process were evaluated and optimized using response surface methodology (RSM) for the first time. The chosen operating parameters were: reaction temperature, initial pH of the reaction mixture and TiO2 P-25 photocatalyst loading. Escherichia coli concentration, after 90 minutes irradiation of UV-A light, was selected as the response. Twenty sets of photocatalytic disinfection experiments were conducted by adjusting operating parameters at five levels using the central composite design. Based on the experimental data, a semi-empirical expression was established and applied to predict the response. Analysis of variance revealed a strong correlation between predicted and experimental values of the response. The optimum values of the reaction temperature, initial pH of the reaction mixture and photocatalyst loading were found to be 40.3 °C, 5.9 g/L, and 1.0 g/L, respectively. Under the optimized conditions, E. coli concentration was observed to reduce from 10(7) to about 11 CFU/mL during the photocatalytic process. Moreover, all these results showed the great significance of the RSM in developing high performance processes for photocatalytic water disinfection.