SrFe0.6Cu0.3Ti0.1O3-δ透氧膜反应器中甲烷部分氧化反应工艺及膜稳定性考察

doi:10.3969/j.issn.0438-1157.2014.05.015

化工学报

• 催化、动力学与反应器 • 上一篇下一篇

SrFe_0.6Cu_0.3Ti_0.1O_3-δ透氧膜反应器中甲烷部分氧化反应工艺及膜稳定性考察

张恒¹, 王婷婷¹, 聂毅², 张香平², 林维明³

1 曲阜师范大学化学与化工学院, 山东曲阜 273165;
2 中国科学院过程工程研究所, 北京 100190;
3 华南理工大学化学与化工学院, 广东广州 510640

收稿日期:2013-12-27 修回日期:2014-02-04 出版日期:2014-05-05 发布日期:2014-05-05
通讯作者: 张恒
基金资助:
国家重点基础研究发展计划项目（2013CB733506）；山东省自然科学基金项目（ZR2012BQ015）。

Investigation of performance of SrFe_0.6Cu_0.3Ti_0.1O₃_-_δ mixed conducting membrane for partial oxidation of methane to syngas

ZHANG Heng¹, WANG Tingting¹, NIE Yi², ZHANG Xiangping², LIN Weiming³

1 School of Chemistry and Chemical Engineering, Qufu Normal University, Qufu 273165, Shandong, China;
2 Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
3 School of Chemical and Energy Engineering, South China University of Technology, Guangzhou 510640, Guangdong, China

Received:2013-12-27 Revised:2014-02-04 Online:2014-05-05 Published:2014-05-05
Supported by:
supported by the National Basic Research Program of China(2013CB733506) and the Natural Science Foundation of Shandong Province (ZR2012BQ0151122).

摘要/Abstract

摘要： 采用SrFe_0.6Cu_0.3Ti_0.1O₃_-δ混合导体透氧膜组装成膜催化反应器，进行甲烷部分氧化制合成气反应，考察了反应温度、空速、催化剂粒径等条件的影响，并分析了反应气氛引起的透氧膜结构变化情况。结果表明，在膜反应器内，催化反应与透氧过程存在相互制约和相互促进的关系。在膜反应器内进行甲烷部分氧化反应后，透氧膜的两侧表面均发生蚀刻现象，结晶度显著降低，反应侧蚀刻现象较为严重，膜表面形成了疏松的多孔层，反应气氛使膜表面晶体结构发生了较大改变，Sr容易从钙钛矿结构中析出并与CO₂结合形成SrCO₃，Sr的析出导致组成不平衡，促进了钙钛矿结构分解及其他物相的产生。

关键词: 甲烷, 合成气, 透氧, 混合导体, 钙钛矿, 稳定性

Abstract: SrFe_0.6Cu_0.3Ti_0.1O₃_-δ membrane was used to install a membrane reactor for partial oxidation of methane to syngas. The influences of temperature, space velocity and catalyst particle size on the reaction were studied, and the change of the phase structure of the membrane was analyzed. The interaction between the oxygen permeating process and the partial oxidation reaction caused different reaction performance in membrane reactor compared with fixed bed reactor. The crystallinity of both sides of the SrFe_0.6Cu_0.3Ti_0.1O₃_-δ membrane declined significantly after the catalytic reaction. The decomposition of the perovskite structure and the formation of SrCO₃ and other phases were found in the reaction-side surface of the membrane, along with the emergence of loose porous morphology.

Key words: methane, syngas, oxygen permeation, mixed conductor, perovskite, stability

中图分类号:

TQ174

张恒, 王婷婷, 聂毅, 张香平, 林维明. SrFe_0.6Cu_0.3Ti_0.1O_3-δ透氧膜反应器中甲烷部分氧化反应工艺及膜稳定性考察[J]. 化工学报, DOI: 10.3969/j.issn.0438-1157.2014.05.015.

ZHANG Heng, WANG Tingting, NIE Yi, ZHANG Xiangping, LIN Weiming. Investigation of performance of SrFe_0.6Cu_0.3Ti_0.1O₃_-_δ mixed conducting membrane for partial oxidation of methane to syngas[J]. CIESC Journal, DOI: 10.3969/j.issn.0438-1157.2014.05.015.

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SrFe_0.6Cu_0.3Ti_0.1O_3-δ透氧膜反应器中甲烷部分氧化反应工艺及膜稳定性考察

Investigation of performance of SrFe_0.6Cu_0.3Ti_0.1O₃_-_δ mixed conducting membrane for partial oxidation of methane to syngas

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SrFe0.6Cu0.3Ti0.1O3-δ透氧膜反应器中甲烷部分氧化反应工艺及膜稳定性考察

Investigation of performance of SrFe0.6Cu0.3Ti0.1O3-δ mixed conducting membrane for partial oxidation of methane to syngas

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SrFe_0.6Cu_0.3Ti_0.1O_3-δ透氧膜反应器中甲烷部分氧化反应工艺及膜稳定性考察

Investigation of performance of SrFe_0.6Cu_0.3Ti_0.1O₃_-_δ mixed conducting membrane for partial oxidation of methane to syngas