物理化学学报 >> 2001, Vol. 17 >> Issue (03): 201-205.doi: 10.3866/PKU.WHXB20010303

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用MS-PSR技术研究甲烷部分氧化反应的引发过程

季亚英;李文钊;徐恒泳;陈燕馨   

  1. 中国科学院大连化学物理研究所，大连　116023
  • 收稿日期:2000-07-04 修回日期:2000-10-20 发布日期:2001-03-15
  • 通讯作者: 李文钊 E-mail:wzli@ms.dicp.ac.cn

Study on the Ignition Process for the Catalytic Partial Oxidation of Methane to Synthesis Gas by MS-TPSR Technique

Ji Ya-Ying;Li Wen-Zhao;Xu Heng-Yong;Chen Yan-Xin   

  1. Dalian Institute of Chemical Physics, Chinese Academy of Sciences,Dalian　116023
  • Received:2000-07-04 Revised:2000-10-20 Published:2001-03-15
  • Contact: Li Wen-Zhao E-mail:wzli@ms.dicp.ac.cn

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摘要： 借助质谱程序升温表面反应(MSTPSR)技术研究了NiO/悛睞l2O3、700 ℃ H2还原 后的Ni0/悛睞l2O3和添加Pt的NiO/悛睞l2O3催化剂(分别记为NiO、Ni0和PtNiO)上甲烷 部分氧化反应(POM)的引发行为.结果表明，在CH4＋O2气氛下NiO和Ni0具有相同的引发行为 ， Ni0在反应气氛下首先被氧化为NiO.在低于760 ℃时， CH4和O2在NiO上发生深度氧化反 应生成H2O和CO2，在770 ℃开始逐渐引发POM反应. PtNiO在520 ℃左右就能引发POM反应 .在流化床反应器中PtNiO催化剂500 ℃左右引发POM反应，并且具有与Ni0基本相同的反应 性能，因此添加Pt有利于氧化镍还原为Ni0，从而降低了POM反应的引发温度.

关键词: 甲烷部分氧化, 合成气, 流化床, Ni催化剂

Abstract: The ignition processes for the catalytic partial oxidation of methane( POM) to synthesis gas over the oxidized nickel, metallic nickel as well as Pta dded oxidized nickel catalysts (represented as NiO, Ni0 and PtNiO, respectivel y) were studied by temperatureprogrammed surface reaction (TPSR)technique. The results showed that the ignition behavior for POM on NiO was almost similar to that on Ni0 in the reacting atmosphere of CH4 and O2, Ni0 was first oxidized to NiO, then the deep oxidation of methane took place on NiO at T< 760 ℃. POM gr adually initiated at ～ 770 ℃ on Ni0 and NiO catalysts, however, even at ～ 520 ℃ could POM rapidly take place on PtNiO catalyst. the catalytic performance of POM initiated on PtNiO catalyst at about 500 ℃ in a fluidized bed was the same as that on Ni0, which indicated that the addition of Pt was beneficial to t he reduction of NiO to active Ni0, therefore the addition of Pt reduced the init ial temperature for POM.

Key words: Partial oxidation of methane, Synthesis gas, Fluidized bed, Ni cat alyst