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甲烷部分氧化制合成气反应中催化剂积炭的研究(英文)

MECHANISM STUDY OF CARBON DEPOSITION ON A Ni/Al2O3 CATALYST DURING PARTIAL OXIDATION OF METHANE TO SYNGAS

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【作者】 严前古吴廷华李基涛罗春容翁维正杨乐夫万惠霖

【Author】 Yan Qiangu; Wu Tinghua; Li Jitao; Luo Chunrong; Weng Weizeng; Yang Lefu; Wan Huilin; ( State Key Laboratory for Physical Chemistly of the Solid Surface Department of Chemistry Xiamen University Xiamen, Fujian 361005; Department of Chemistry Zhejiang Norma

【机构】 固体表面物理化学国家重点实验室!厦门大学化学系福建厦门361005浙江师范大学化学系浙江金华!321004固体表面物理化学国家重点实验室!厦门大学

【摘要】 Ni/Al催化剂上甲烷部分氧化制合成气反应是在固定床流动反应装置上进行的。考察了催化剂的床层温度、反应压力、空速和原料气配比对催化剂积炭产生的影响。实验结果表明,积炭速率随催化剂床层温度的升高而降低,当温度低于70℃时,积炭速率骤增:积炭总是发生在催化剂床层的下段;若空速超过3.0×10-1,积炭速率随空速增加而明显降低。从FTIR实验结果可知,吸附在Ni/Al催化剂表面上的CO,一部分歧化生成了CO和C。综上所述,催化剂表面积炭主要来源于以下两个反应: 2CO→C+CO,CO+H = C+H

【Abstract】 The performance of a Ni/A12O3 catalyst for the oxidation of methane to syngas has been investigated in a fixed bed flow reactor. The effects of temperature in catalyst bed, reactor pressure, space velocity and Ch4/O@ ratio on carbon deposition over the catalyst were examined. The results revealed that the rate of carbon deposition decreased with the increase of catalyst bed temperature and increased When the bed temperature decreased, especially, the rate could be accelerated at temperatures below 700℃. The carbon deposition always occurred on the catalyst located in the down stream region of the bed during reaction. When the space velocity exceeded a certain value (3.0×l05 h-1), the fate of carbon deposition would decrease significantly with the increase of the space velocity. The FTIR results of CO adsorption over the Ni/Al2O3 catalyst implied that the adsorbed CO might be a precursor of CO disproportionation to CO2 and carbon. Based on these results, it is proposed that the carbon deposits may be mainly produced from the Boudouaral reaction f 2CO = C+CO2 and/or the heterogeneous water-gas reaction; CO+H2 = C+H2O.

【基金】 the Ministry of Science and Technology of China (No. G1999022408) and the Doctoral Foundation from the Ministry of Education.
  • 【文献出处】 Journal of Natural Gas Chemistry ,天然气化学杂志(英文版) , 编辑部邮箱 ,2000年02期
  • 【分类号】TQ426
  • 【被引频次】5
  • 【下载频次】87
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