Redox conversion of methane with Fe2O3-CaTixM1-xO3 composite oxides for hydrogen and liquid fuel co-production

doi:10.3969/j.issn.0438-1157.2014.07.035

Abstract

Abstract: Structural, crystalline phase, and redox properties of three composite oxides with a general formula of Fe₂O₃-CaTi_xM₁_-xO₃ were investigated. Integral and differential bed reactors were used to investigate methane partial oxidation and water-splitting reactions. In their oxidized form, all three composites consisted of orthorhombic perovskite phase and hematite phase. Activities for methane partial oxidation followed the sequence: Fe₂O₃-CaTi_0.85Ni_0.15O₃ > Fe₂O₃-CaTi_0.85Co_0.15O₃ > Fe₂O₃-CaTi_0.85Fe_0.15O₃. Fixed bed results indicated that Fe₂O₃-CaTi_0.85Ni_0.15O₃ was capable of converting 96% CH₄ with syngas yield of 71%. Steam to hydrogen conversion in water-splitting was 40%. ASPEN Plus^® simulations indicated that Fe₂O₃-CaTi_0.85Ni_0.15O₃, when used in the hybrid solar-redox process, could signficantly enhance methane utilization efficiency for liquid fuel and H₂ co-production.

Key words: perovskite composite, methane, catalytic oxidation, hydrogen production

摘要： 利用固相法合成了3种钙钛矿型复合氧化物Fe₂O₃-CaTi_xM₁_-xO₃，研究了其结构、晶型和氧化还原活性。在固定床反应器中考察了该氧化物对两步法甲烷催化氧化制合成气及水分解制氢的活性及选择性。X射线衍射结果表明3种钙钛型复合氧化物均由正交晶系钙钛矿相和赤铁矿相组成。3种钙钛矿复合氧化物对甲烷的氧化活性顺序为Fe₂O₃-CaTi_0.85Ni_0.15O₃ >Fe₂O₃-CaTi_0.85Co_0.15O₃ >Fe₂O₃-CaTi_0.85Fe_0.15O₃。固定床反应结果表明，以Fe₂O₃-CaTi_0.85Ni_0.15O₃为氧载体催化剂，CH₄转化率可达96%，CO和H₂产率达71%，同时水分解反应的转化率为40%。利用Aspen Plus^®对Fe₂O₃-CaTi_0.85Ni_0.15O₃在混合太阳能氧化还原过程的效率及合成油和H₂产率进行了模拟。模拟计算结果证明基于复合氧化物的混合太阳能氧化还原过程可以有效提高CH₄利用率。

关键词: 钙钛矿型复合氧化物, 甲烷, 催化氧化, 制氢

CLC Number:

O643.36

CHEN Yanguang, HE Feng, DAGA Shivalik, LI Fanxing. Redox conversion of methane with Fe₂O₃-CaTi_xM₁_-xO₃ composite oxides for hydrogen and liquid fuel co-production[J]. CIESC Journal, 2014, 65(7): 2741-2750.

陈彦广, 何峰, Daga Shivalik, 李凡星. 钙钛矿型复合氧化物对甲烷的部分氧化及在混合太阳能氧化还原过程的应用[J]. 化工学报, 2014, 65(7): 2741-2750.

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Redox conversion of methane with Fe₂O₃-CaTi_xM₁_-xO₃ composite oxides for hydrogen and liquid fuel co-production

钙钛矿型复合氧化物对甲烷的部分氧化及在混合太阳能氧化还原过程的应用

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