Catalyst-modified perovskite hollow fiber membrane for oxidative coupling of methane

doi:10.1016/j.cjche.2021.11.012

中国化学工程学报 ›› 2022, Vol. 41 ›› Issue (1): 412-419.DOI: 10.1016/j.cjche.2021.11.012

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Catalyst-modified perovskite hollow fiber membrane for oxidative coupling of methane

Jian Song^1,2, Claudia Li³, Shao Zhang², Xiuxia Meng¹, Bo Meng¹, Jaka Sunarso³

1 Department of Chemical Engineering, Shandong University of Technology, Zibo 255049, China;
2 State Key Laboratory of Separation Membranes and Membrane Processes, Department of Chemical Engineering, Tiangong University, Tianjin 300387, China;
3 Research Centre for Sustainable Technologies, Faculty of Engineering, Computing and Science, Swinburne University of Technology, Jalan Simpang Tiga, 93350 Kuching, Sarawak, Malaysia

收稿日期:2021-08-01 修回日期:2021-10-20 出版日期:2022-01-28 发布日期:2022-02-25
通讯作者: Jaka Sunarso,E-mail addresses:barryjakasunarso@yahoo.com,jsunarso@swinburne.edu.my
基金资助:
The authors gratefully acknowledge the research funding provided by the National Natural Science Foundation of China (21805206, 22179073).

Catalyst-modified perovskite hollow fiber membrane for oxidative coupling of methane

Jian Song^1,2, Claudia Li³, Shao Zhang², Xiuxia Meng¹, Bo Meng¹, Jaka Sunarso³

1 Department of Chemical Engineering, Shandong University of Technology, Zibo 255049, China;
2 State Key Laboratory of Separation Membranes and Membrane Processes, Department of Chemical Engineering, Tiangong University, Tianjin 300387, China;
3 Research Centre for Sustainable Technologies, Faculty of Engineering, Computing and Science, Swinburne University of Technology, Jalan Simpang Tiga, 93350 Kuching, Sarawak, Malaysia

Received:2021-08-01 Revised:2021-10-20 Online:2022-01-28 Published:2022-02-25
Contact: Jaka Sunarso,E-mail addresses:barryjakasunarso@yahoo.com,jsunarso@swinburne.edu.my
Supported by:
The authors gratefully acknowledge the research funding provided by the National Natural Science Foundation of China (21805206, 22179073).

摘要/Abstract

摘要： The catalytic oxidative coupling of methane (OCM) to C₂ hydrocarbons (C₂H₆ and C₂H₄) represents one of the most effective ways to convert natural gas to more useful products, which can be performed effectively using La_0.6Sr_0.4Co_0.2Fe_0.8O_3-δ (LSCF) perovskite hollow fiber membrane microreactor. In this work, the effects of adding a thin BaCe_0.8Gd_0.2O_3-δ (BCG) catalyst film onto the inner LSCF fiber surface as the OCM catalyst and a porous Ba_0.5Sr_0.5Co_0.8Fe_0.2O_3-δ (BSCF) perovskite layer onto the outer LSCF surface to improve the oxygen permeation were evaluated. Between 700 ℃ and 1000 ℃, methane conversion increased in the order of uncoated, BCG and BSCF-coated, and BCG-coated LSCF hollow fiber while C₂-selectivity and C₂-yield increased in the order of BCG and BSCF-coated, uncoated, and BCG-coated LSCF hollow fiber. Oxygen permeation flux at the same temperature range, on the other hand, was enhanced in the order of uncoated, BCG-coated, and BCG and BSCF-coated LSCF hollow fiber. This finding demonstrates the complex interplay between oxygen permeation and OCM performance. The BCG and BSCF-coated hollow fiber was also subjected to thermal cycles between 850 ℃ and 900 ℃ for up to 175 hours during which the fiber showed minor degradation in oxygen permeation fluxes and relatively stable OCM performance.

关键词: Hollow fiber, Membrane reactor, Oxidative coupling of methane (OCM), Perovskite

Abstract: The catalytic oxidative coupling of methane (OCM) to C₂ hydrocarbons (C₂H₆ and C₂H₄) represents one of the most effective ways to convert natural gas to more useful products, which can be performed effectively using La_0.6Sr_0.4Co_0.2Fe_0.8O_3-δ (LSCF) perovskite hollow fiber membrane microreactor. In this work, the effects of adding a thin BaCe_0.8Gd_0.2O_3-δ (BCG) catalyst film onto the inner LSCF fiber surface as the OCM catalyst and a porous Ba_0.5Sr_0.5Co_0.8Fe_0.2O_3-δ (BSCF) perovskite layer onto the outer LSCF surface to improve the oxygen permeation were evaluated. Between 700 ℃ and 1000 ℃, methane conversion increased in the order of uncoated, BCG and BSCF-coated, and BCG-coated LSCF hollow fiber while C₂-selectivity and C₂-yield increased in the order of BCG and BSCF-coated, uncoated, and BCG-coated LSCF hollow fiber. Oxygen permeation flux at the same temperature range, on the other hand, was enhanced in the order of uncoated, BCG-coated, and BCG and BSCF-coated LSCF hollow fiber. This finding demonstrates the complex interplay between oxygen permeation and OCM performance. The BCG and BSCF-coated hollow fiber was also subjected to thermal cycles between 850 ℃ and 900 ℃ for up to 175 hours during which the fiber showed minor degradation in oxygen permeation fluxes and relatively stable OCM performance.

Key words: Hollow fiber, Membrane reactor, Oxidative coupling of methane (OCM), Perovskite

Jian Song, Claudia Li, Shao Zhang, Xiuxia Meng, Bo Meng, Jaka Sunarso. Catalyst-modified perovskite hollow fiber membrane for oxidative coupling of methane[J]. 中国化学工程学报, 2022, 41(1): 412-419.

Jian Song, Claudia Li, Shao Zhang, Xiuxia Meng, Bo Meng, Jaka Sunarso. Catalyst-modified perovskite hollow fiber membrane for oxidative coupling of methane[J]. Chinese Journal of Chemical Engineering, 2022, 41(1): 412-419.

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Catalyst-modified perovskite hollow fiber membrane for oxidative coupling of methane

Catalyst-modified perovskite hollow fiber membrane for oxidative coupling of methane

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