Partial oxidation of methane to syngas with air by lattice oxygen transfer over ZrO2-modified Ce-Fe mixed oxides
Partial oxidation of methane to syngas with air by lattice oxygen transfer over ZrO2-modified Ce-Fe mixed oxides
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ZrO2 改性 Ce-Fe 混合氧化物上晶格氧转移将甲烷部分氧化为合成气
DOI：
10.1016/j.cej.2011.08.006
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发表时间：
2011-09
影响因子：
15.1
通讯作者：
Yan, Dongxia
中科院分区：
文献类型：
--
作者：
Li, Kongzhai;Wang, Hua;Wei, Yonggang;Yan, Dongxia
研究了以ZrO 2为助剂的Ce-Fe复合氧化物对甲烷部分氧化制合成气的催化性能。结果表明，适量的ZrO 2通过提高Ce-Fe材料中氧空位的浓度和改善游离Fe 2 O3的分散性，增强了Ce-Fe材料与CeO 2之间的相互作用，从而提高了Ce-Fe材料的甲烷部分氧化活性。但是，ZrO 2的大量添加会导致CeO 2和Fe 2 O3从Ce-Fe固溶体中分离，从而降低合成气的选择性。在所测试的样品中，Ce-Fe-Zr（0.05）样品表现出最好的催化性能（具有高的甲烷转化率和合成气选择性）。尽管严重烧结，Ce-Fe-Zr（0.05）氧化物在用于连续生产合成气的重复氧化还原过程（甲烷还原/空气再氧化）期间呈现高催化稳定性。这可能是由于循环后复合氧化物表面氧空位浓度增加，提高了晶格氧的迁移率，抵消了材料烧结对甲烷部分氧化催化活性的影响。
Catalytic performance of Ce–Fe mixed oxides promoted with ZrO2was investigated for methane partial oxidation to syngas via gas–solid reactions. The results showed that moderate amounts of ZrO2could strongly enhance the interaction between iron and cerium oxides via increasing the oxygen vacancy concentration and improving the dispersion of free Fe2O3, which improved the activity of Ce–Fe material for methane partial oxidation. However, heavy loading of ZrO2would lead to a phase segregation of CeO2and Fe2O3from the Ce–Fe solid solution, resulting in a decrease in syngas selectivity. Among the tested samples, Ce–Fe–Zr (0.05) sample showed the best catalytic performance (with both high methane conversion and syngas selectivity). Despite severe sintering, the Ce–Fe–Zr (0.05) oxides presented high catalytic stability during the repetitive redox process (methane reduction/air re-oxidation) for the continuous production of syngas. This property should be attributed to the increased oxygen vacancy concentration on the mixed oxides after cycling, which could improve the lattice oxygen mobility, counteracting the native effect of material sintering on the catalytic activity for methane partial oxidation.
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