Low-Temperature Synthesis and Catalytic Activity of Cobalt Ferrite in Nitrous Oxide (N2O) Decomposition Reaction

Cobalt ferrite (CoFe2O4) nanoparticles were synthesized and investigated as a catalyst in the reaction of nitrous oxide (N2O) decomposition. Cobalt ferrite was synthesized by solid–phase interaction at 1100 °C and by preliminary mechanochemical activation in a roller-ring vibrating mill at 400 °C. The nanoparticles were characterized by X-ray diffraction (XRD), synchronous thermal analysis (TG and DSC) and scanning electron microscopy (SEM). A low-temperature nitrogen adsorption/desorption test was used to evaluate the catalytic activity of the cobalt ferrite nanoparticles. Correlations between the structure and catalytic properties of the catalysts are reported. The highest catalytic activity of CoFe2O4 in the reaction of nitrous oxide decomposition was 98.1% at 475 °C for cobalt ferrite obtained by mechanochemical activation.

Kinetic modeling of nitrous oxide decomposition on Fe-ZSM-5 in the presence of nitric oxide based on parameters obtained from first-principles calculations

A variety of experiments for the N2O decomposition over Fe-ZSM-5 catalysts have been simulated in the presence and absence of small amounts of nitric oxide and water vapor.

N2O Decomposition over Fe-ZSM-5: A Systematic Study in the Generation of Active Sites

We have carried out a systematic investigation of the critical activation parameters (i.e., final temperature (673–1273 K), atmosphere (He vs. O2/He), and final isothermal hold (1 min–15 h) on the generation of “α-sites”, responsible for the direct N2O decomposition over Fe-ZSM-5 (Fe content = 1200–2300 ppm). The concentration of α-sites was determined by (ia) transient response of N2O and (ib) CO at 523 K, and (ii) temperature programmed desorption (TPD) following nitrous oxide decomposition. Transient response analysis was consistent with decomposition of N2O to generate (i) “active” α-oxygen that participates in the low-temperature CO→CO2 oxidation and (ii) “non-active” oxygen strongly adsorbed that is not released during TPD. For the first time, we were able to quantify the formation of α-sites, which requires a high temperature (>973) treatment of Fe-ZSM-5 in He over a short period of time (<1 h). In contrast, prolonged high temperature treatment (1273 K) and the presence of O2 in the feed irreversibly reduced the amount of active sites.

Effect of Water Molecule on Photo-Assisted Nitrous Oxide Decomposition over Oxotitanium Porphyrin: A Theoretical Study

Water vapor has generally been recognized as an inhibitor of catalysts in nitrous oxide (N2O) decomposition because it limits the lifetime of catalytic reactors. Oxygen produced in reactions also deactivates the catalytic performance of bulk surface catalysts. Herein, we propose a potential catalyst that is tolerant of water and oxygen in the process of N2O decomposition. By applying density functional theory calculations, we investigated the reaction mechanism of N2O decomposition into N2 and O2 catalyzed by oxotitanium(IV) porphyrin (TiO-por) with interfacially bonded water. The activation energies of reaction Path A and B are compared under thermal and photo-assisted conditions. The obtained calculation results show that the photo-assisted reaction in Path B is highly exothermic and proceeds smoothly with the low activation barrier of 27.57 kcal/mol at the rate determining step. The produced O2 is easily desorbed from the surface of the catalyst, requiring only 4.96 kcal/mol, indicating the suppression of catalyst deactivation. Therefore, TiO-por is theoretically proved to have the potential to be a desirable catalyst for N2O decomposition with photo-irradiation because of its low activation barrier, water resistance, and ease of regeneration.

Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)+

Infrared multiple-photon dissociation spectroscopy has been applied to study Ptn(N2O)+ (n = 1–8) clusters which represent entrance-channel complexes on the reactive potential energy surface for nitrous oxide decomposition on platinum.