Coordination-Controlled Catalytic Activity of Cobalt Oxides for Ozone Decomposition.

Nowadays, it is still elusive and challenging to discover the active sites of cobalt (Co) cations in different coordination structures, though Co-based oxides show their great potency in catalytic ozone elimination for air cleaning. Herein, different Co-based oxides are controllably synthesized including hexagonal wurtzite CoO-W with Co2+ in tetrahedral coordination (CoTd2+) and CoAl spinel with dominant CoTd2+, cubic rock salt CoO-R with Co2+ in octahedral coordination (CoOh2+), MgCo spinel with dominant Co3+ in octahedral coordination (CoOh3+), and Co3O4 with mixed CoTd2+ and CoOh3+. The valences are proved by X-ray photoelectron spectroscopy, and the coordinations are verified by X-ray absorption fine structure analysis. The ozone decomposition performances are CoOh3+ ∼ CoOh2+ ≫ CoTd2+, and CoOh3+ and CoOh2+ show a lower apparent activation energy of ∼42-44 kJ/mol than CoTd2+ (∼55 kJ/mol). In specific, MgCo shows the highest decomposition efficiency of 95% toward 100 ppm ozone at a high space velocity of 1,200,000 mL/gh, which still retains at 80% after a long-term running of 36 h at room temperature. The high activity is explained by the d-orbital splitting in the octahedral coordination, favoring the electron transfer in ozone decomposition reactions, which is also verified by the simulation. These results show the promising prospect of the coordination tuning of Co-based oxides for highly active ozone decomposition catalysts.

Abatement of dichloromethane with high selectivity over defect-rich MOF-derived Ru/TiO2 catalysts.

The regulation of oxygen vacancies and Ru species using metal-organic frameworks was synergically adopted in a rational design to upgrade Ru/TiO2 catalysts, which are highly active for the catalytic oxidation of dichloromethane (DCM) with less undesired byproducts. In this work, Ru/M-TiO2 and Ru/N-TiO2 catalysts were synthesized by the pyrolysis of MIL-125 and NH2-MIL-125 incorporated with Ru, the existence of Ru nanoclusters and nanoparticles was detected by XAFS, respectively, and the catalytic performance was analyzed comprehensively. Complete oxidation of DCM was obtained at ∼290 °C over Ru/M-TiO2 and Ru/N-TiO2 catalysts, while Ru/N-TiO2 showed quite less monochloromethane (MCM) and higher CO2 yields, and better dechlorination capacity in oxidation. The distinction comes down to that the easier desorption of chlorine could be achieved over Ru4+ which act as the main activated adsorption sites for DCM in Ru/N-TiO2, compared to oxygen vacancies that serve as the main dissociation sites in Ru/M-TiO2. Additionally, Ru/N-TiO2 exhibited superior stability and excellent resilience in moisture. An in situ DRIFTS experiment further indicated the different DCM catalytic degradation process as well as the reaction mechanism over the as-prepared catalysts.

Aqueous Strippable Polymer Coating for Highly Efficient Primary Radioactive Uranium Decontamination with Versatility on Diversified Surface.

The decontamination of radioactive materials on the surfaces of nuclear facilities has generated large quantities of waste from the rapid development of the nuclear industry, posing a potential threat globally. Strippable coating has been employed for some time to remove radioactive contamination due to its high performance and removability, flexibility, and compatibility with various substrates. Herein, an aqueous strippable coating based on an adsorbent/polyvinyl alcohol (PVA) polymer was developed to remove radioactive uranium from stainless-steel surfaces that showed greater decontamination than that of DeconGel, with an efficiency of 87.2% for 5 g/L uranium and 95.5% for 22.5 g/L uranium, along with a high repeatability and better mechanical properties. Furthermore, the prepared coating was versatile and could be applied to a range of substrate surfaces (lacquered, aluminum, glass, plastic, and ceramic), with outstanding performance ranging from 79.2 to 95.4% for 1 g/L uranium. The prepared coating could also be applied through brushing or spraying to horizontal or vertical substrates. The exceptional performance could be due to the synergistic effect of the introduction of ethylene diamine tetra-acetic acid disodium salt (EDTA-2Na) as a chelating agent and the nano-adsorbent CaCO3/TiO2.