| 焙烧气氛对Ru/Al2O3催化剂上甲烷部分氧化制合成气反应性能的影响 |
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| 引用本文： | 郑好转,王梅柳,华卫琦,翁维正,伊晓东,黄传敬,万惠霖.焙烧气氛对Ru/Al2O3催化剂上甲烷部分氧化制合成气反应性能的影响[J].催化学报,2011,32(1):93-99. |
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| 作者姓名： | 郑好转 王梅柳 华卫琦 翁维正 伊晓东 黄传敬 万惠霖 |
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| 作者单位： | 1厦门大学固体表面物理化学国家重点实验室, 醇醚酯化工清洁生产国家工程实验室, 化学化工学院化学系, 福建厦门 361005; 2烟台万华聚氨酯股份有限公司, 山东烟台 264002 |
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| 基金项目： | 国家自然科学基金，国家重点基础研究发展计划(973计划，福建省重大科技专项 |
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| 摘 要： | 采用气相色谱、质谱和原位时间分辨红外光谱等技术对空气和Ar气氛中焙烧的Ru/Al2O3催化剂样品上甲烷部分氧化(POM)制合成气反应进行了跟踪,并采用化学吸附、X射线衍射、拉曼光谱和H2-程序升温还原等技术对催化剂进行了表征.结果表明,在Ru/Al2O3-Air上POM反应出现振荡现象,而在Ru/Al2O3-Ar上则可...
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| 关 键 词： | 钌 氧化铝 焙烧气氛 甲烷 部分氧化 合成气 振荡 |
| 收稿时间： | 2010-06-25 |
Effect of Calcination Atmospheres on the Performance of Ru/Al_2O_3 Catalyst for Partial Oxidation of Methane to Syngas |
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| ZHENG Haozhuan,WANG Meiliu,HUA Weiqi,WENG Weizheng,YI Xiaodong,HUANG Chuanjing,WAN Huilin.Effect of Calcination Atmospheres on the Performance of Ru/Al_2O_3 Catalyst for Partial Oxidation of Methane to Syngas[J].Chinese Journal of Catalysis,2011,32(1):93-99. |
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| Authors: | ZHENG Haozhuan WANG Meiliu HUA Weiqi WENG Weizheng YI Xiaodong HUANG Chuanjing WAN Huilin |
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| Institution: | 1State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China; 2Yantai Wanhua Polyurethanes Co., Ltd., Yantai 264002, Shandong, China |
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| Abstract: | The catalytic performance for partial oxidation of methane (POM) to syngas over the Ru/Al2O3 catalyst calcined in air (Ru/Al2O3-Air) and Ar (Ru/Al2O3-Ar) was studied. Steady-state reactivity was observed on the Ru/Al2O3-Ar sample, whereas oscillations in CH4, CO, H2, CO2, and H2O were observed on the Ru/Al2O3-Air sample. Comparative studies using CO and O2 chemisorption, X-ray diffraction, Raman, and temperature-programmed reduction (TPR) techniques were carried out in order to elucidate the property-structure relationship of the samples. The Ru dispersion on Ru/Al2O3-Air was only 1%, whereas that on Ru/Al2O3-Ar was about 9%. The significant difference in the Ru dispersion on the two samples is the major factor affecting the POM reaction. Two types of Ru species, RuO2 species weakly interacting with Al2O3 and the Ru-O-Al species strongly interacting with the support, were identified by H2-TPR experiments on the fresh catalyst. The former species could be easily reduced by H2 (below 200 °C), while the latter can only be reduced by H2 at above 700 °C. During the POM reaction at above 600 °C, the RuO2 species were in the metal state, whereas the Ru-O-Al species could undergo cyclic redox transformation. Such transformation is responsible for the oscillation on Ru/Al2O3-Air sample. |
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| Keywords: | ruthenium alumina calcination atmosphere methane partial oxidation syngas oscillation |
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