N2O is a greenhouse gas and a candidate oxidant. Volatile organic pollutants (VOCs) have caused great harm to the atmospheric ecological environment. Developing the technique utilizing N2O as the oxidant to oxidize VOCs to realize the collaborative purification has significant importance and practical value for N2O emission control and VOC abatement. Therefore, the study of N2O catalytic oxidation of tert-butanol based on zeolite catalysts was carried out. A series of molecular sieves, including FER, MOR, ZSM-5, Y, and BEA, were selected as the catalyst objects, and the 1.5% wt Fe and Co were, respectively, loaded on the zeolite catalysts via the impregnation method. It was found that the catalytic performance of BEA was the best among the molecular sieves. Comparing the catalytic performance of Fe-BEA under different load gradients (0.25~2%), it was found that 1.5% Fe-BEA possessed the best catalytic activity. A series of characterization methods showed that Fe3+content in 1.5% Fe-BEA was the highest, and more active sites formed to promote the catalytic reaction. The α-O in the reaction eventually oxidized tert-butanol to CO2over the active site. The Co mainly existed in the form of Co2+cations over Co-BEA samples; the 2% Co-BEA possessing higher amounts of Co2+exhibited the highest activity among the prepared Co-BEA samples.
Shi Jin,Zhang Zihao,Chen Mingxia,Zhang Zhixiang,Shangguan Wenfeng,Gu Shunchao,Shin-ichi Hirano
Fe-BEA catalysts are active for the NH3-SCR of NO. For industrial application, a binder should be added to the Fe-BEA catalysts to make them tightly adhere to the monoliths. The addition of alumina and zirconia as binders to the Fe-BEA led to a different effect on NO conversion. The catalytic activity of the mixed samples was evaluated by the temperature programmed procedure in a flow-reactor system, and the mechanism was analyzed via SEM, BET, XRD and XPS. It was found that larger iron particles were formed by the migration of parent iron particles in the Fe-BEA catalyst with alumina. This led to the increase of Fe 3+ magnitude and iron cluster, enhancing the abilities of NO oxidation and storage. Accordingly, the SCR activity increased slightly in low temperature but decreased sharply in high temperature. For the Fe-BEA with zirconia sample, NO oxidation and storage abilities decreased due to the less iron clusters. The increase of Fe 3+ magnitude resulted in higher catalytic oxidation ability, which gave rise to little change in the SCR activity compared with the Fe-BEA.