铈修饰铁基复合载氧体用于化学链甲烷部分氧化重整制合成气研究

张军伟; 黄戒介; 房倚天; 王志青; 余钟亮

铈修饰铁基复合载氧体用于化学链甲烷部分氧化重整制合成气研究

1.
中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西太原 030001;
2.
中国科学院大学, 北京 100049

基金项目: 中国科学院战略性先导科技专项（XDA07050100）；山西省青年科技研究基金（2013021007-2）

详细信息

通讯作者:
黄戒介，研究员，Tel/Fax：0351-2021137，E-mail：huangjj@sxicc.ac.cn

中图分类号: TE646
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出版历程
- 收稿日期: 2013-07-23
- 修回日期: 2013-09-09
- 刊出日期: 2014-02-28

Partial oxidation reforming of methane to synthesis gas by chemical-looping using CeO₂-modified Fe₂O₃ as oxygen carrier

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China;
2.
University of Chinese Academy of Sciences, Beijing 100049, China

摘要

摘要: 以Al₂O₃为惰性载体，利用共沉淀法制备了CeO₂-Fe₂O₃-Al₂O₃复合载氧体，并对载氧体进行了XRD、SEM表征。在固定床反应器中，考察了程序升温、恒温、多循环等操作条件下，载氧体对甲烷部分氧化重整的反应性能。程序升温实验结果表明，在相同温度下，CeO₂含量为30%的载氧体与不含CeO₂的载氧体对比，CH₄转化率、H₂和CO选择性均提高。在恒温实验中，含有CeO₂的两种载氧体，CH₄转化率、H₂和CO选择性上也都明显高于不含CeO₂的载氧体，当反应时间小于1 200 s时，无积炭发生。三种载氧体经过15次循环后，CeO₂含量为30%的载氧体表现出最佳的循环特性。多循环实验中，当反应温度850 ℃、反应时间945 s时，CH₄最大转化率达到91.53%、H₂的最大选择性达到86.36%、CO的最大选择性达到85.12%、H₂与CO的最佳平均物质的量比为2.03。XRD谱图显示，经过多次循环后，三种载氧体的物相没有发生变化，载氧体表现出了很好的稳定性能。
- 化学链 /
- 载氧体 /
- 甲烷 /
- 合成气 /
- 循环
Abstract: The CeO₂/Fe₂O₃ oxygen carriers were prepared by co-precipitation method and their characterization was carried out using X-ray diffraction (XRD) and scanning electron microscope (SEM). The partial oxidation reforming of methane was tested in a fixed-bed at different operating conditions. The temperature programming results show that 30% CeO₂-modified Fe₂O₃ has rather better effect than pure Fe₂O₃; the conversion of CH₄, the selectivity of H₂ and CO are greatly improved. Same results have been observed in isothermal experiments. As the reaction time is less than 1 200 s, there is no carbon deposit formed. After 15 cycles, 30% CeO₂-modified Fe₂O₃ has the best cycling performance at 850 ℃ and the reaction time of 945 s. The conversion of CH₄ reaches to 91.53%, the selectivity of H₂ and CO reach to 86.36% and 85.12%, respectively and the H₂/CO mol ratio in syngas is 2.03. The species of substance in oxygen carriers has no obvious change after 15 cycles.
- chemical-looping /
- oxygen carrier /
- methane /
- synthesis gas /
- cycle

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