物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2014年
5期
957-964
,共8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%浸渍法%载体
錳氧化物%鈀%臭氧%催化分解%浸漬法%載體
맹양화물%파%취양%최화분해%침지법%재체
Manganese oxide%Pal adium%Ozone%Catalytic decomposition%Impregnation method%Support
在γ-Al2O3载体上用等体积浸渍法浸渍Pd、MnOx活性组分,然后涂覆于堇青石基体上制备Pd-MnOx/γ-Al2O3整体式催化剂.分别用 X 射线衍射(XRD)、H2-程序升温还原(H2-TPR)、低温 N2吸附-脱附及 X 射线光电子能谱(XPS)对制备的催化剂进行表征.研究了Pd、MnOx浸渍顺序对催化剂活性、氧化还原性能及织构性质的影响.实验结果表明, Pd、MnOx共浸渍较分别浸渍制备的催化剂活性好, Pd 和 MnOx之间存在一定的协同作用.考察了不同载体如La-Al2O3、SiO2、γ-Al2O3和Zr-Al2O3对催化剂活性、氧化还原性能、织构性质及表面电子性能的影响.研究表明,以La-Al2O3或SiO2为载体的催化剂活性最好,即,14°C时O3转化率为82%,完全转化温度为36°C.γ-Al2O3载体次之, Zr-Al2O3载体较差.不同载体制备的催化剂中 MnOx的氧化还原性能顺序为: Pd-MnOx/SiO2>Pd-MnOx/La-Al2O3>Pd-MnOx/γ-Al2O3>Pd-MnOx/Zr-Al2O3.
在γ-Al2O3載體上用等體積浸漬法浸漬Pd、MnOx活性組分,然後塗覆于堇青石基體上製備Pd-MnOx/γ-Al2O3整體式催化劑.分彆用 X 射線衍射(XRD)、H2-程序升溫還原(H2-TPR)、低溫 N2吸附-脫附及 X 射線光電子能譜(XPS)對製備的催化劑進行錶徵.研究瞭Pd、MnOx浸漬順序對催化劑活性、氧化還原性能及織構性質的影響.實驗結果錶明, Pd、MnOx共浸漬較分彆浸漬製備的催化劑活性好, Pd 和 MnOx之間存在一定的協同作用.攷察瞭不同載體如La-Al2O3、SiO2、γ-Al2O3和Zr-Al2O3對催化劑活性、氧化還原性能、織構性質及錶麵電子性能的影響.研究錶明,以La-Al2O3或SiO2為載體的催化劑活性最好,即,14°C時O3轉化率為82%,完全轉化溫度為36°C.γ-Al2O3載體次之, Zr-Al2O3載體較差.不同載體製備的催化劑中 MnOx的氧化還原性能順序為: Pd-MnOx/SiO2>Pd-MnOx/La-Al2O3>Pd-MnOx/γ-Al2O3>Pd-MnOx/Zr-Al2O3.
재γ-Al2O3재체상용등체적침지법침지Pd、MnOx활성조분,연후도복우근청석기체상제비Pd-MnOx/γ-Al2O3정체식최화제.분별용 X 사선연사(XRD)、H2-정서승온환원(H2-TPR)、저온 N2흡부-탈부급 X 사선광전자능보(XPS)대제비적최화제진행표정.연구료Pd、MnOx침지순서대최화제활성、양화환원성능급직구성질적영향.실험결과표명, Pd、MnOx공침지교분별침지제비적최화제활성호, Pd 화 MnOx지간존재일정적협동작용.고찰료불동재체여La-Al2O3、SiO2、γ-Al2O3화Zr-Al2O3대최화제활성、양화환원성능、직구성질급표면전자성능적영향.연구표명,이La-Al2O3혹SiO2위재체적최화제활성최호,즉,14°C시O3전화솔위82%,완전전화온도위36°C.γ-Al2O3재체차지, Zr-Al2O3재체교차.불동재체제비적최화제중 MnOx적양화환원성능순서위: Pd-MnOx/SiO2>Pd-MnOx/La-Al2O3>Pd-MnOx/γ-Al2O3>Pd-MnOx/Zr-Al2O3.
Pd-MnOx/γ-Al2O3 catalysts were prepared by impregnating Pd and MnOx on γ-Al2O3 supports, using an incipient wetness impregnation method, and then coating on a cordierite substrate to obtain monolithic catalysts. The catalysts were characterized using X-ray diffraction (XRD), temperature-programmed reduction of H2 (H2-TPR), low-temperature N2 adsorption-desorption measurements, and X-ray photoelectron spectroscopy (XPS). The effects of the Pd and MnOx impregnation order on the catalytic activity, redox performance, textural properties, and surface electronic characteristics of the catalysts were studied. The experimental results showed that the activity of the catalyst co-impregnated with Pd and MnOx on γ-Al2O3 was better than that of the catalyst impregnated sequentially with Pd and MnOx. A synergetic effect was observed between Pd and MnOx on the Pd-MnOx/γ-Al2O3 catalysts for ozone decomposition. The effects of various supports on catalytic activity, redox performance, textural properties, and surface electron characteristics of the catalysts were also investigated. The results indicated that the catalytic activities of Pd-MnOx/La-Al2O3 and Pd-MnOx/SiO2 catalysts were the best; ozone conversion reached 82% at 14 °C and ozone was completely decomposed at 36 ° C. The activity of the Pd- MnOx/γ- Al2O3 catalyst was second better, but the activity of the Pd-MnOx/Zr-Al2O3 catalyst was poor. The support clearly affects the reducibility of PdO and MnOx. The redox performances of MnOx impregnated on different supports fol owed the order:Pd-MnOx/SiO2>Pd-MnOx/La-Al2O3>Pd-MnOx/γ-Al2O3>Pd-MnOx/Zr-Al2O3.