Development and performance of CeO2 supported BaCoO3−δ perovskite for chemical looping steam methane reforming

合成气 化学链燃烧 蒸汽重整 制氢 甲烷 化学 钙钛矿(结构) 催化作用 氧气 二氧化碳重整 部分氧化 甲烷转化炉 脱氢 无机化学 水煤气变换反应 化学工程 有机化学 工程类
作者
Haoran Ding,Yonggang Jin,Stephen C. Hawkins,Liqi Zhang,Cong Luo
出处
期刊:Fuel Processing Technology [Elsevier BV]
卷期号:239: 107546-107546 被引量:11
标识
DOI:10.1016/j.fuproc.2022.107546
摘要

Chemical looping steam methane reforming (CL-SMR) is a promising approach to co-production of syngas and hydrogen, and the reactivity of oxygen carriers is crucial in the performance of CL-SMR. In this study, CeO 2 supported BaCoO 3-δ oxygen carriers with different component distributions (labeled as dry-mix, sol-gel, co-sol-gel samples) were prepared and evaluated in CL-SMR. The BaCoO 3-δ was loosely attached on CeO 2 in the dry-mix sample, resulting in a high resistance to oxygen mobility and a low gas production. The co-sol-gel sample possessed impurities of Co 3 O 4 , BaCO 3 and BaCeO 3 , which decreased reaction capacity and enhanced the secondary reaction of methane decomposition, leading to an excessive H 2 /CO ratio of syngas and coke formation. The contact of perovskite and CeO 2 in sol-gel sample favors the synergistic effect of perovskite and CeO 2, where the H 2 /CO ratio was close to the ideal value of 2 at 850 °C with the produced syngas and hydrogen reaching 4.57 mol/kg and 1.47 mol/kg, respectively. In situ Diffuse Reflectance Infrared Fourier Transform spectroscopy was employed to investigate the reaction mechanism of partial oxidation of methane, indicating that CH 4 is gradually dehydrogenated and partially oxidized by lattice oxygen, and the conversion of -O-CH 3 into -CHO and H 2 is the rate-controlling step. • CeO 2 /BaCoO 3-δ oxygen carriers with three different chemical distributions were prepared. • The uniform perovskite layer on CeO 2 support was essential for oxygen supply and reactivity. • A proper temperature could make a balance between reactivity and oxygen mobility. • The conversion of -O-CH 3 → –CHO is the rate controlling step in POM stage.
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