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稀土等碱性助剂对甲烷部分氧化制合成气整体式Ni/-γAl2O3催化剂性能的影响

Partial Oxidation of Methane to Syngas over Monolithic Ni/γ-Al2O3 Catalyst——Effects of Rare Earths and Other Basic Promoters

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【作者】 马迪梅大江李璇龚茂初陈耀强

【Author】 Ma Di,Mei Dajiang,Li Xuan,Gong Maochu,Chen Yaoqiang~* (College of Chemistry,Sichuan University,Chengdu 610064,China)

【机构】 四川大学化学学院四川大学化学学院 四川成都610064四川成都610064

【摘要】 制备了整体式Ni/-γAl2O3和添加稀土等碱性助剂的整体式Ni/-γAl2O3催化剂。研究了温度、烷氧比、空速和助剂等因素对甲烷部分氧化反应性能的影响,并利用XRD和TPR对催化剂进行了表征。结果表明,催化剂活性随着温度的升高而增加;CH4转化率随着烷氧比的增加而降低;当空速为1×105h-1时,整体式催化剂的催化性能最佳。添加碱性助剂Ce,La,Na,Sr均有利于改善催化剂的还原性能,提高催化剂的活性。其中添加稀土Ce,La可使副反应CH4+2 O2→CO2+2H2O完全被抑制,从而使H2选择性达到100%。

【Abstract】 A series of monolithic Ni/γ-Al2O3 catalysts with and without basic promoters(Na,Sr,La,Ce) were prepared.The partial oxidation of methane(POM) to syngas was carried out in a continuous-flow and fixed-bed reactor.The influence of reaction conditions(temperature,CH4/O2 ration,space velocity) on the performance of catalyst was investigated.The results demonstrate that at high space velocity of 1×105 h-1,optimal CH4 conversion can be obtained.Effects of promoters such as Na,Sr,Ce,La were also investigated,and the catalyst samples were characterized by means of temperature-programmed reduction(TPR) and XRD techniques.XRD suggests that the addition of promoters has no influence on the crystal structure of Ni/γ-Al2O3 catalyst.The results show that the addition of small amount of promoters improves the reducibility and activity of the catalyst.The side reaction CH4 + 2 O2 → CO2+2H2O,has been fully restrained and 100% H2 selectivity has been achieved when Ce,La are promoted respectively.

【基金】 国家重点基础研究规划项目(G1999022400)资助
  • 【文献出处】 中国稀土学报 ,Journal of the Chinese Rare Earth Society , 编辑部邮箱 ,2006年03期
  • 【分类号】O643.36;TE665.3
  • 【被引频次】18
  • 【下载频次】272
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