Insight into phase structure-dependent soot oxidation activity of K/MnO2 catalyst

Abstract

In the present study, two nanosized MnO2 with β and δ phase structures and potassium loaded MnO2 catalysts with varied K loading amounts (denoted as K/MnO2) were prepared. Temperature programmed oxidation and isothermal reactions in loose contact modes were employed to examine the soot oxidation activity of the as-prepared catalysts. Characterization results show that as compared with β-MnO2, δ-MnO2 has larger surface area and higher content of hydroxyl groups. Upon K loading, abundant hydroxyl groups in δ-MnO2 effectively sequestrate K cation to form bound K species and free K species are available only at K loading above 3.0 wt.%. In contrast, the majority of K species present as free state in β-MnO2 even at a K loading of 1.0 wt.% due to its very low hydroxyl group content. The O2 temperature-programmed desorption (O2-TPD) demonstrates that the catalysts with free K species exhibit strong ability in activating gaseous O2, whereas the catalysts only having bound K display minor O2 activation capability. As a result, despite of slightly lower activity of β-MnO2 than δ-MnO2, the K/β-MnO2 catalysts exhibit substantially higher activities than K/δ-MnO2 catalysts with identical K loadings. The finding in this study clearly demonstrates that for MnO2 based catalysts, the enhancement of catalytic activity for soot oxidation is highly K loading amount dependent and the dependency is strongly associated with the phase structure of MnO2.