催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2014年
11期
1883-1891
,共9页
任成军%周丽娜%尚鸿燕%陈耀强
任成軍%週麗娜%尚鴻燕%陳耀彊
임성군%주려나%상홍연%진요강
锰氧化物%钯%臭氧%催化分解%制备方法
錳氧化物%鈀%臭氧%催化分解%製備方法
맹양화물%파%취양%최화분해%제비방법
Manganese oxide%Palladium%Ozone%Catalytic decomposition%Preparation method
分别用溶胶凝胶法和分步沉淀法制备了MnOx+γ-Al2O3和MnOx/γ-Al2O3,用等体积浸渍法将等量的Pd(NO3)2分别浸渍于其上,再将它们分别涂覆于堇青石上,得到不同物理化学性质的整体式催化剂,并采用X射线衍射、X射线光电子能谱、程序升温还原和低温N2吸附-脱附等技术对催化剂进行表征.结果表明,制备方法和MnOx焙烧温度明显影响催化剂中MnOx的物相、表面Mn物种和表面活性氧物种的分布及织构性质.活性测试结果表明,两种制备方法得到的催化剂于16-90 oC,380000-580000 h-1条件下均可将0.6μL·L-1 O3完全分解;尤其是溶胶凝胶法制备的Pd/γ-Al2O3+MnOx/γ-Al2O3催化剂分解O3活性较好,催化剂表面Mn2+:Mn3+:Mn4+=1.7:1:3(mol).
分彆用溶膠凝膠法和分步沉澱法製備瞭MnOx+γ-Al2O3和MnOx/γ-Al2O3,用等體積浸漬法將等量的Pd(NO3)2分彆浸漬于其上,再將它們分彆塗覆于堇青石上,得到不同物理化學性質的整體式催化劑,併採用X射線衍射、X射線光電子能譜、程序升溫還原和低溫N2吸附-脫附等技術對催化劑進行錶徵.結果錶明,製備方法和MnOx焙燒溫度明顯影響催化劑中MnOx的物相、錶麵Mn物種和錶麵活性氧物種的分佈及織構性質.活性測試結果錶明,兩種製備方法得到的催化劑于16-90 oC,380000-580000 h-1條件下均可將0.6μL·L-1 O3完全分解;尤其是溶膠凝膠法製備的Pd/γ-Al2O3+MnOx/γ-Al2O3催化劑分解O3活性較好,催化劑錶麵Mn2+:Mn3+:Mn4+=1.7:1:3(mol).
분별용용효응효법화분보침정법제비료MnOx+γ-Al2O3화MnOx/γ-Al2O3,용등체적침지법장등량적Pd(NO3)2분별침지우기상,재장타문분별도복우근청석상,득도불동물이화학성질적정체식최화제,병채용X사선연사、X사선광전자능보、정서승온환원화저온N2흡부-탈부등기술대최화제진행표정.결과표명,제비방법화MnOx배소온도명현영향최화제중MnOx적물상、표면Mn물충화표면활성양물충적분포급직구성질.활성측시결과표명,량충제비방법득도적최화제우16-90 oC,380000-580000 h-1조건하균가장0.6μL·L-1 O3완전분해;우기시용효응효법제비적Pd/γ-Al2O3+MnOx/γ-Al2O3최화제분해O3활성교호,최화제표면Mn2+:Mn3+:Mn4+=1.7:1:3(mol).
MnOx+γ-Al2O3 and MnOx/γ-Al2O3 catalysts were prepared by the sol-gel and sequential precipitation methods, respectively. The same amount of Pd was loaded on these catalysts by incipient wetness impregnation. The two Pd-MnOx/γ-Al2O3 catalysts with different physicochemical properties were coated on cordierite. The catalysts were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, and N2 adsorption-desorption measurement. The preparation method and calcination temperature of MnOx have significant impact on the crys-talline phase of MnOx, MnOx species and active oxygen species, and textural properties of the cata-lysts. The experimental results showed that 0.60 μL?L-1 of ozone was completely decomposed on these catalysts in the temperature range of 16 to 90 °C at space velocities from 380000 to 580000 h-1. In particular, the activity for O3 decomposition was excellent on the Pd/MnOx+Pd/γ-Al2O3 cata-lyst that used MnOx prepared by the sol-gel method. Mnn+is beneficial for O3 decomposition, and Mn2+, Mn3+, and Mn4+were presented in a mole ratio of 1.7:1:3 on the surface of the catalyst.