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1.天津大学化工学院,绿色合成与转化教育部重点实验室,天津 300072
2.佛山(华南)新材料研究院, 广东 佛山 528000
Received:18 February 2020,
Revised:2020-06-21,
Online First:03 November 2020,
Published:05 November 2020
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苏迎辉, 郑浩, 张磊, 曾亮. LaMn1-x-yFexCoyO3-δ钙钛矿载氧体用于化学链部分氧化[J]. 化工学报, 2020, 71(11): 5265-5277 DOI: 10.11949/0438-1157.20200158.
SU Yinghui, ZHENG Hao, ZHANG Lei, ZENG Liang. LaMn1-x-yFexCoyO3-δ perovskite based oxygen carriers for chemical looping partial oxidation[J]. CIESC Journal, 2020, 71(11): 5265-5277 DOI: 10.11949/0438-1157.20200158.
苏迎辉, 郑浩, 张磊, 曾亮. LaMn1-x-yFexCoyO3-δ钙钛矿载氧体用于化学链部分氧化[J]. 化工学报, 2020, 71(11): 5265-5277 DOI: 10.11949/0438-1157.20200158. DOI:
SU Yinghui, ZHENG Hao, ZHANG Lei, ZENG Liang. LaMn1-x-yFexCoyO3-δ perovskite based oxygen carriers for chemical looping partial oxidation[J]. CIESC Journal, 2020, 71(11): 5265-5277 DOI: 10.11949/0438-1157.20200158. DOI:
采用溶胶-凝胶法制备了B位Fe和Co共取代的LaMn
1-
x
-
y
Fe
x
Co
y
O
3-
δ
钙钛矿型复合氧化物,并用于化学链甲烷部分氧化制合成气。X射线衍射(XRD)结果表明Fe和Co均进入了LaMnO
3
的晶格形成钙钛矿晶相,活性和稳定性测试表明LaMn
1/3
Fe
1/3
Co
1/3
O
3-
δ
载氧体具有最佳的化学链甲烷部分氧化性能。CH
4
程序升温还原(CH
4
-TPR)表征发现LaMn
1/3
Fe
1/3
Co
1/3
O
3-
δ
具有比LaBO
3
(B=Co, Mn, Fe)更高的甲烷活化能力和晶格氧迁移性能。甲烷恒温脉冲反应(CH
4
-pulse reaction)进一步证实了B位离子的协同作用可以提高LaBO
3
(B=Co, Mn, Fe)的表面反应速率。程序升温氢气还原(H
2
-TPR)表明,LaMn
1/3
Fe
1/3
Co
1/3
O
3-
δ
中晶格氧具有适中的氧化还原能力,适合用于化学链甲烷部分氧化。
LaMn
1-
x
-
y
Fe
x
Co
y
O
3-
δ
perovskite-type composite oxides co-substituted with B-site Fe and Co were prepared by the sol-gel method
and used for the chemical looping partial oxidation of methane to syngas. The XRD results suggest that Fe and Co were incorporated into the lattice of LaMnO
3
and formed perovskite phase. Reactivity and stability tests show that LaMn
1/3
Fe
1/3
Co
1/3
O
3-
δ
oxygen carrier has the best reaction performance. CH
4
-TPR results indicate that LaMn
1/3
Fe
1/3
Co
1/3
O
3-
δ
has higher methane activation and lattice oxygen migration rates than those of LaBO
3
(B=Co
Mn
Fe). CH
4
-pulse reaction further
confirms that the synergistic effect of B-site ion substitution can improve the surface reaction rate of LaBO
3
(B=Co
Mn
Fe). H
2
-TPR results show that the lattice oxygen in LaMn
1/3
Fe
1/3
Co
1/3
O
3-
δ
has moderate redox capacity
which is suitable for partial oxidation of methane.
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