Although LaMnO3 perovskite oxide has been reported to exhibit low activity in NO direct decomposition into N2 and O2, doping Ga or In at the Mn site of La(Ba)MnO3 has been found effective of increasing the activity for NO direct decomposition into N 2 and O2. The activity of NO decomposition increased in the order Ba>Sr>Ca for the La site dopant, and In>Ga for the Mn site. Among the investigated dopants and compositions, the highest N2 yield was achieved with La0.7Ba0.3Mn0.8In 0.2O3. On this catalyst, NO conversion increased with increasing reaction temperature, and at 1123 K, NO conversion into N 2 and O2 attained values of 75 and 41%, respectively. The high yield of N2 and O2 was maintained for 12 h. Coexistence of oxygen decreased the N2 yield with PO2 -0.53; however, a N2 yield of 15% could be sustained even at 10% coexisting O2 at 1073 K. The NO decomposition rate increased with increasing NO partial pressure and obeyed with PNO 1.31. O2 temperature-programmed desorption measurements showed that oxygen desorption was greatly enhanced by In doping at the Mn site. NO TPD also showed that the amount of NO adsorbed greatly increased with In doping. Therefore, improved activity of NO decomposition with In substitution seems to be caused by the weakening adsorption of oxygen and the increased adsorption of NO. IR measurements of adsorbed NO also suggest that the major adsorption species at high temperature was NO3- and it seems likely that NO decomposition proceeds after removal of NO3 - and/or oxygen. N2O direct decomposition on La 0.7Ba0.3Mn0.8In0.2O3 was further studied. It was found that La0.7Ba0.3Mn 0.8In0.2O3 is highly active in the direct decomposition of N2O even under the coexistence of O2. Therefore, decomposition of NO on La0.7Ba0.3Mn 0.8In0.2O3 may proceed via N2O as the intermediate species.
All Science Journal Classification (ASJC) codes
- Physical and Theoretical Chemistry