Catalytic behaviors of chloromethane combustion over the metal-modified ZSM-5 zeolites with diverse SiO2/Al2O3 ratios
Catalytic behaviors of chloromethane combustion over the metal-modified ZSM-5 zeolites with diverse SiO2/Al2O3 ratios
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DOI：
10.1016/j.molcata.2014.11.019
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发表时间：
2015-03
影响因子：
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通讯作者：
Runduo Zhang;Bo Zhang;Zhaoyuan Shi;Ning Liu;Biaohua Chen
中科院分区：
文献类型：
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作者：
Runduo Zhang;Bo Zhang;Zhaoyuan Shi;Ning Liu;Biaohua Chen
采用传统湿法浸渍法制备了一系列不同摩尔比的SiO2/Al2O3(30, 107) M/ZSM-5 (M = Co, Fe, Ce, Mn)催化剂，并通过XRD、BET、H2-TPR、NH3-TPD、XPS等手段进行了表征，并进行了氯甲烷催化燃烧活性测试。即使在浸渍各种金属成分后，ZSM-5的特征结构也基本保持。所研究的催化剂在 1500 ppm CH3Cl、10% O2 和 15,000 h−1 GHSV 的气氛下实现的催化活性遵循 Co/ZSM-5-30、Ce/ZSM-5-30 > Co/ZSM-5-107、Ce/ZSM-5-107、Fe/ZSM-5-30、 Mn/ZSM-5-30 > Mn/ZSM-5-107、Fe/ZSM-5-107 > H-ZSM-5-30 > H-ZSM-5-107。二元 Co/ZSM-5-30 和 Ce/ZSM-5-30 在 400 °C 下表现出令人满意的 CH3Cl 转化率（87% 和 95%），同时 CO 产率较低（9.6% 和 16%），这归因于所制备的沸石催化剂具有优异的氧化还原性能（由负载金属组分的化学性质决定）和强酸性性能（通过 Al 同晶取代改性）。
A series of M/ZSM-5 (M = Co, Fe, Ce, and Mn) catalysts with different molar ratios of SiO2/Al2O3(30, 107) was prepared via a traditional wetness impregnation, and further characterized by XRD, BET, H2-TPR, NH3-TPD, and XPS as well as activity test for the catalytic combustion of chloromethane. Characteristic structure of ZSM-5 is basically maintained even after impregnating the various metallic components. Catalytic activities achieving under an atmosphere of 1500 ppm CH3Cl, 10% O2, and GHSV of 15,000 h−1of the investigated catalysts follow a trend of Co/ZSM-5-30, Ce/ZSM-5-30 > Co/ZSM-5-107, Ce/ZSM-5-107, Fe/ZSM-5-30, Mn/ZSM-5-30 > Mn/ZSM-5-107, Fe/ZSM-5-107 > H-ZSM-5-30 > H-ZSM-5-107. The binary Co/ZSM-5-30 and Ce/ZSM-5-30 show the satisfactory conversions of CH3Cl (87% and 95%) associated with a low yield of CO (9.6% and 16%) at 400 °C, owing to the excellent redox properties (determined by the chemical nature of the loaded metallic components) and strong acidic properties (modified by Al isomorphic substitution) of the as-prepared zeolitic catalysts.