In the present study,two nanosized MnO_(2)with β and δ phase structures and potassium loaded MnO_(2)catalysts with varied K loading amounts (denoted as K/MnO_(2)) were prepared.Temperature programmed oxidation and i...In the present study,two nanosized MnO_(2)with β and δ phase structures and potassium loaded MnO_(2)catalysts with varied K loading amounts (denoted as K/MnO_(2)) 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-MnO_(2),δ-MnO_(2)has larger surface area and higher content of hydroxyl groups.Upon K loading,abundant hydroxyl groups in δ-MnO_(2)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-MnO_(2)even at a K loading of 1.0 wt.%due to its very low hydroxyl group content.The O_(2)temperature-programmed desorption (O_(2)-TPD) demonstrates that the catalysts with free K species exhibit strong ability in activating gaseous O_(2),whereas the catalysts only having bound K display minor O_(2)activation capability.As a result,despite of slightly lower activity of β-MnO_(2)than δ-MnO_(2),the K/β-MnO_(2)catalysts exhibit substantially higher activities than K/δ-MnO_(2)catalysts with identical K loadings.The finding in this study clearly demonstrates that for MnO_(2)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 MnO_(2).展开更多
基金supported by the National Key Research and Development Program of China (No.2020YFC1807003)National Natural Science Foundation of China (Nos.21976086and 22002059)Open Fund of the State Key Lab of Pollution Control and Resource Reuse Research of China (No.PCRR-ZZ-202105)。
文摘In the present study,two nanosized MnO_(2)with β and δ phase structures and potassium loaded MnO_(2)catalysts with varied K loading amounts (denoted as K/MnO_(2)) 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-MnO_(2),δ-MnO_(2)has larger surface area and higher content of hydroxyl groups.Upon K loading,abundant hydroxyl groups in δ-MnO_(2)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-MnO_(2)even at a K loading of 1.0 wt.%due to its very low hydroxyl group content.The O_(2)temperature-programmed desorption (O_(2)-TPD) demonstrates that the catalysts with free K species exhibit strong ability in activating gaseous O_(2),whereas the catalysts only having bound K display minor O_(2)activation capability.As a result,despite of slightly lower activity of β-MnO_(2)than δ-MnO_(2),the K/β-MnO_(2)catalysts exhibit substantially higher activities than K/δ-MnO_(2)catalysts with identical K loadings.The finding in this study clearly demonstrates that for MnO_(2)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 MnO_(2).
