高等学校化学学报 ›› 2002, Vol. 23 ›› Issue (11): 2106.

• 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(Ⅱ)──催化剂组成与反应条件对催化剂性能的影响

魏俊梅, 徐柏庆, 孙科强, 李晋鲁, 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:2001-08-26 出版日期:2002-11-24 发布日期:2002-11-24
  • 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@mai.ltsinghua.edu.cn E-mail:bqxu@mai.ltsinghua.edu.cn
  • 基金资助:

    国家自然科学基金(批准号:20073023);国家杰出青年基金(批准号:20125310)资助

CO2 Reforming of CH4 over Ni Supported on Nano-ZrO2(Ⅱ)── Effect of Catalyst Composition and Reaction Conditions on Catalytic Reactivity

WEI Jun-Mei, XU Bo-Qing, SUN Ke-Qiang, LI Jin-Lu, ZHU Qi-Ming   

  1. Department of Chemistry, State Key Laboratory of C1 Chemistry & Technology, Tsinghua University, Beijing 100084, China
  • Received:2001-08-26 Online:2002-11-24 Published:2002-11-24

摘要: 研究了粒径为15~18nm的纳米ZrO2-AS负载Ni催化剂对CO2重整CH4制合成气的催化性能,结果表明,Ni/ZrO2-AS催化剂对重整反应的超常稳定催化作用不受Ni含量的影响,但当Ni质量分数低于10%时,催化剂活性随Ni含量增加而显著上升,此后,CH4和CO2的转化逐渐接近其热力学平衡值.高空速虽然降低了反应物的转化率,但可得到更高的时空产率.各种表征数据揭示,Ni/ZrO2在结构上有别于传统的负载型催化剂,可看成是由尺寸相当(10~20nm)的纳米金属Ni和纳米ZrO2形成的纳米复合物催化剂.

关键词: 二氧化碳重整甲烷, 合成气, 纳米ZrO2, Ni催化剂, 纳米复合物催化剂

Abstract: Ni "supported" nano-zirconia catalyst(named as Ni/ZrO2-AS) was extremely stable for CO2 reforming of CH4 to syngas. In the present work, the effects of the Ni loading(5%-32%), reaction temperature(923-1 123 K) and space velocity[GHSV=104-105 mL/(h·g-cat)] were extensively studied. While the catalytic stability of Ni/ZrO2-AS catalysts seemed not significantly affected by the Ni loading, the increase of the loading up to 10% improved effectively the catalyst activity at 1 030 K. In the reactions over the catalysts with higher Ni loadings, the conversions of the reactants approached their values for thermodynamic equilibrium. The increase of the feed space velocity led to a decrease of the reactant conversions, but to an increase of the space time yield of syngas product. TPO measurement of the carbon deposition showed that every nickel atoms in the catalysts survived dynamically two carbon atoms on the average. TPR/TPD and TEM characterizations revealed that Ni/ZiOr2-AS catalysts were different in structure from conventional metal catalysts supported on porous oxides; they were nano-composites of size-comparable metallic Ni and ZrO2 nanocrystals( 10-20 nm). The catalytic stability of Ni catalysts in Ni/ZrO2-AS system is most probably connected with the nature of the nanoacomposite structures.

Key words: CO2 reforming of CH4, Syngas, Nano-zirconia, Ni catalyst, Nanacomposite catalyst

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