RESUMEN

Formaldehyde decomposition is not only an attractive method for hydrogen production, but also a potential approach for gaseous formaldehyde removal. In this research, we prepare some assembled organoruthenium through coordination reaction between Ru(p-Cymene)Cl2 and bridge-linking ligands. It is a creative approach for Ru(p-Cymene)Cl2 conversion into heterogeneous particles. The rigidity of bridge-linking ligand enables assembled organoruthenium to have highly ordered crystalline structure, even show clear crystal lattice with spacing of 0.19 nm. XPS shows the N-Ru bond are formed between bridge-linking ligand and Ru(p-Cymene)Cl2 . The assembled organoruthenium has high abundant active sites for formaldehyde decomposition at low temperature. The reaction rate could increase linearly with temperature and formaldehyde concentration, with a TOF of 2420 h-1 at 90 °C. It is promising for gaseous formaldehyde decomposition in wet air or nitrogen. Formaldehyde conversion is up to 95 % over Ru-DAPM is 4,4'-diaminodiphenylmethane at 90 °C in air. Gaseous formaldehyde decomposition is a two-steps process under oxygen-free condition. Firstly, formaldehyde dissolve in water, and be converted into hydrogen and formic acid through formaldehyde-water shift reaction. Then intermediate formic acid will further decompose into hydrogen and carbon dioxide. We also find formaldehyde decomposition is a synergetic catalysis process of oxygen and water in moist air. Oxygen is conducive to formic acid desorption and decomposition on the active sites, so assembled organoruthenium exhibit slightly higher conversion for formaldehyde decomposition in moist air. This work proposes a distinctive method for gaseous formaldehyde decomposition in the air, which is entirely different from formaldehyde photocatalysis or thermocatalysis oxidation.

RESUMEN

Large ambient temperature changes (-20->25 °C) bring great challenges to the purification of the indoor pollutant formaldehyde. Within such a large ambient temperature range, we herein report a manganese-based strategy, that is, a mullite catalyst (YMn2O5) + ozone, to efficiently remove the formaldehyde pollution. At -20 °C, the formaldehyde removal efficiency reaches 62% under the condition of 60,000 mL gcat-1 h-1. As the reaction temperature is increased to -5 °C, formaldehyde and ozone are completely converted into CO2, H2O, and O2, respectively. Such a remarkable performance was ascribed to the highly reactive oxygen species generated by ozone on the YMn2O5 surface based on the low temperature-programed desorption measurements. The in situ infrared spectra showed the intermediate product carboxyl group (-COOH) to be the key species. Based on the superior performance, we built a consumable-free air purifier equipped with mullite-coated ceramics. In the simulated indoor condition (25 °C and 30% relative humidity), the equipment can effectively decompose formaldehyde (150 m3 h-1) without producing secondary pollutants, rivaling a commercial removal efficiency. This work provides an air purification route based on the mullite catalyst + ozone to remove formaldehyde in an ambient temperature range (-20->25 °C).

Asunto(s)

RESUMEN

Doping with noble metal ions or doping with nitrogen has been attempted to prepare TiO2 that reacts even in visible light. In this study, TiO2 was doped with nitrogen and various metal ions instead of noble metals. The TiO2 photocatalysts doped with metal ions (Fe, Ag, Ni) and nitrogen were prepared by a sol-gel method. Their physicochemical properties were characterized and their photocatalytic activities were investigated under visible light irradiation. In TiO2 doped with metal ions and nitrogen, the light absorption region was extended to visible light. The photoluminescence intensity was much greater in N/Ni/TiO2 than in N/Ag/TiO2 and N/Fe/TiO2. The photolysis activities of N/Ni/TiO2 were the highest in formaldehyde decomposition and methylene blue decomposition. The sterilization efficiency of N/Ni/TiO2 was the highest in the evaluation test for the inhibition of the proliferation of Pseudomonas aeruginosa. The bandgap of N/Ni/TiO2 was 2.4 eV, which was significantly lower than that of anatase TiO2 (3.2 eV). The N/Ni/TiO2 had a much higher optical intensity than other metal ion-doped TiO2, so it was highly active under visible light irradiation.