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尿素加入量对水热合成法制备Mn取代六铝酸盐催化剂的影响

Effect of Amounts of Urea on Mn-substituted Hexaaluminate Catalysts Prepared by Hydrothermal Synthesis

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【作者】 徐金光田志坚王军威徐云鹏徐竹生林励吾

【Author】 XU Jin-Guang1, TIAN Zhi-Jian 1*, WANG Jun-Wei1, XU Yun-Peng1, XU Zhu-Sheng1, LIN Li-WU 1,2 (1. Research Laboratory of Natural Gas Chemical Engineering and Application; 2. State Key Laboratory of Catalytic Basis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China)

【机构】 中国科学院大连化学物理研究所天然气化工与应用催化研究室中国科学院大连化学物理研究所天然气化工与应用催化研究室 催化基础国家重点实验室大连116023

【摘要】 采用以尿素水解为基础的水热合成法制备了 Mn取代的镧六铝酸盐催化剂 .研究了尿素加入量对所制备催化剂的化学组成、相结构、孔结构及甲烷催化燃烧活性的影响 . n(尿素 ) / n( M+ ) (其中 M+为带单位正电荷的金属离子 )为 1.0时 ,Mn2 +离子沉淀不完全 ,所得催化剂甲烷催化燃烧活性较低 .n(尿素 ) / n( M+ )增加到 2 .0时 ,Mn2 +离子沉淀完全 ,催化剂中六铝酸盐相增加 ,平均孔直径增大 ,甲烷催化燃烧活性提高 .n(尿素 ) / n( M+ )再增加至 4 .0时 ,比表面积降低 ,六铝酸盐相减少 ,平均孔直径降低 ,甲烷催化燃烧活性下降 .n(尿素 ) / n( M+ )为 2 .0时 ,所制备的催化剂在 780℃及反应生成水蒸汽下运行 10 0 h,催化剂比表面积及甲烷燃烧活性都保持稳定 .

【Abstract】 Mn-substituted hexaaluminate catalysts were prepared by hydrothermal synthesis based on hydrolysis of urea. The effects of amounts of urea[n(Urea)/ n(M+), M+ is metal cation with a single charge] added on chemical composition, phase, pore structure and methane combustion activity of the LaMnAl 11O 19-α catalysts were investigated. When n(Urea)/n(M+)=1.0, Mn 2+ ions did not precipitated completely and the activity of the catalyst for methane combustion was low. With n(Urea)/ n(M+) ratio increasing to 2.0, the activity of catalyst was increased due to more amounts of hexaaluminate phase and larger pore diameter in the catalyst. With increasing of n(Urea)/n(M+) ratio further more, the activity of catalyst was decreased because amounts of hexaaluminate phase in the catalyst were decreased and the pore diameter of the catalyst became smaller. The life test during 100 h the catalyst prepared with n(Urea)/{n(M+)=}2.0 was carried out and the results showed that the activity of the catalyst for methane combustion and the specific surface area of the catalyst were maintained during 100 h life test.

【基金】 国家重点基础研究发展规划项目 (批准号 :G19990 2 2 40 1)资助
  • 【文献出处】 高等学校化学学报 ,Chemical Research In Chinese Universities , 编辑部邮箱 ,2004年01期
  • 【分类号】O643.3
  • 【被引频次】18
  • 【下载频次】334
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