高等学校化学学报

高等学校化学学报 ›› 2002, Vol. 23 ›› Issue (1): 92.

• 研究论文 • 上一篇    下一篇

CO2重整CH4纳米ZrO2负载Ni催化剂的研究(Ⅰ)——与常规载体上Ni催化剂的比较

魏俊梅, 徐柏庆, 李晋鲁, 程振兴, 王亚权, 朱起明   

  1. 清华大学化学系, 一碳化学与化工国家重点实验室, 北京 100084
  • 收稿日期:2000-12-11 出版日期:2002-01-24 发布日期:2002-01-24
  • 通讯作者: 徐柏庆(1961年出生),男,博士,教授,博士生导师,从事多相催化研究.E-mail:bqxu@mail.tsinghua.edu.cn E-mail:bqxu@mail.tsinghua.edu.cn
  • 基金资助:

    国家自然科学基金(批准号:20073023);清华大学重点基础研究基金(批准号:JC1999051)资助

CO2 Reforming of CH4 over Ni Supported on Nano-ZrO2(Ⅰ) Comparison with Conventional Oxide Supported Nickel

WEI Jun-Mei, XU Bo-Qing, LI Jin-Lu, CHENG Zhen-Xing, WANG Ya-Quan, ZHU Qi-Ming   

  1. State Key Laboratory of C1 Chemistry and Technology, Department of Chemistry, Tsinghua University, Beijing 100084, China
  • Received:2000-12-11 Online:2002-01-24 Published:2002-01-24

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摘要： 在Ni负载量相近(约5%)时,比较了由超临界干燥得到的纳米ZrO2-AS为载体制备的Ni/ZrO2-AS与几种常规载体(γ-Al2O3,TiO2,SiO2和ZrO2-CP)负载的Ni催化剂对CO2重整CH4制合成气反应的催化性能.研究结果表明,γ-Al2O3,TiO2,SiO2和ZrO2-CP负载Ni催化剂表现出明显的失活过程,而Ni/ZrO2-AS催化剂在反应200h后活性未下降.“纯ZrO2-AS”载体本身不仅能催化生成合成气的反应,而且活性稳定.TPO测定结果表明,负载在这种活性ZrO2-AS载体上的Ni催化剂具有良好的抗积炭能力.

关键词: 二氧化碳, 甲烷重整, 合成气, 镍催化剂, 纳米ZrO2, 载体效应

Abstract: The catalytic activity and stability of Ni supported on γ-Al2O3, TiO2, SiO2, conventional ZrO2-CP, and nano-ZrO2-AS(15-20 nm) were comparatively studied for CO2 reforming of CH4 to synthesis gas. The Ni loading in these catalysts was limited to 5%(mass fraction) of the supports, and the reaction was performed in a fixed bed flow microreactor at 1030 K with GHSV=2.4×104 mL/(h·g cat). The initial CH4 conversions of the catalysts are in the order of Ni/ γ-Al2O3>Ni/TiO2>Ni/ZrO2-CP> Ni/ZrO2-AS > Ni/SiO2 . Ni catalysts supported on γ-Al2O3, TiO2, ZrO2-CP and SiO2 deactivated rapidly in less than 50h TOS, but Ni/ZrO2-AS catalyst showed no deactivation for longer than 200h. The pure ZrO2-AS also showed a catalytic activity for the reaction and no loss of the activity was observed during50 h on stream at 1073 K. TPOmeasurements demonstrated that carbon deposition on the Ni/ZrO2-AS catalyst was much less and was eliminated at lower temperature than those over the other catalysts. Explanation for the excellent stability of Ni/ZrO2-AS catalyst was given based on the present data. It is suggested that Ni/ZrO2-AS can be better expressed as a nano composite of the Ni and ZrO2-AS, and high percentage of the metal-support perimeter in the composite seems crucial for the long stability of the catalyst.

Key words: Carbon dioxide, Methane reforming, Synthesis gas, Ni catalyst, Nano-zirconia catalyst, Support effect

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