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Effects of Co-substitution on the reactivity of double perovskite oxides LaSrFe2-xCoxO6 for the chemical-looping steam methane reforming
Zhao, Kun1,2,3,4; Chen, Jing1,2,3,5; Li, Haibin1,2,3; Zheng, Anqing1,2,3; He, Fang1,2,3
刊名JOURNAL OF THE ENERGY INSTITUTE
2019-06-01
卷号92期号:3页码:594-603
关键词Chemical looping Methane reforming Double perovskite Synergistic effect Oxygen vacancy
ISSN号1743-9671
DOI10.1016/j.joei.2018.03.013
通讯作者Zheng, Anqing(zhengaq@ms.giec.ac.cn) ; He, Fang(hefang@ms.giec.ac.cn)
英文摘要The double perovskite oxides (DPOs) LaSrFe2-xCoxO6 (x = 0, 0.2, 0.4, 0.6, 0.8) were investigated as oxygen carriers for the chemical looping steam methane reforming (CL-SMR). The fresh oxides were prepared by micro-emulsion method and their physical and chemical properties were characterized by X-ray diffraction, H2-temperature programmed reduction and X-ray photoelectron spectroscopy technologies. Meanwhile, isothermal reactions for methane reforming and steam splitting were carried out in a fixed-bed reactor to determine the influences of Co-substitution on the reactivity of LaSrFe2-xCoxO6. The substitution of metal Co has no obvious effect on the crystal structure of double perovskite, but induces a certain degree of Fe/Co disorder generating oxygen vacancies and/or higher oxidation states of metal cations. Synergistic interaction between surface metal ions, such as (Fe4+/Fe5+-O2--Co2+) and (Fe3+-O2--Co3+), plays a positive effect for the dissociation of methane. The activity may be more likely to be associated with the active oxygen species in connection with Co species on the DPOs surface and abundant of syngas was generated due to the concordant of methane dissociation with the lattice oxygen diffusion. Comprehensively considered, an optimal range of the degree of Co substitution is x = 0.4-0.6 for LaSrFe2-xCoxO6, probably converting 70% of CH4 into CO and H-2 with molar ratio around 2:1. At the reduced states, the ability of DPOs for steam splitting is primarily associated with the oxygen vacancies after oxygen consumption. The substitution of metal Co slightly enhances the hydrogen production capacity and resistance to carbon formation, achieving the average hydrogen yields at 2.89-3.33 mmol/g oxygen carrier and 1.46-1.61 wt% of carbon depositions. (C) 2018 Energy Institute. Published by Elsevier Ltd. All rights reserved.
资助项目National Natural Science Foundation of China[51406208] ; National Natural Science Foundation of China[51406214] ; Science & Technology Research Project of Guangdong Province[2015A010106009]
WOS关键词OXYGEN CARRIER ; HYDROGEN-PRODUCTION ; PARTIAL OXIDATION ; MIXED OXIDES ; PERFORMANCE ; REDUCTION ; GAS ; CATALYST ; COMBUSTION ; STABILITY
WOS研究方向Energy & Fuels
语种英语
出版者ELSEVIER SCI LTD
WOS记录号WOS:000469152800018
资助机构National Natural Science Foundation of China ; Science & Technology Research Project of Guangdong Province
内容类型期刊论文
源URL[http://ir.giec.ac.cn/handle/344007/25133]  
专题中国科学院广州能源研究所
通讯作者Zheng, Anqing; He, Fang
作者单位1.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou, Guangdong, Peoples R China
2.CAS Key Lab Renewable Energy, Beijing, Peoples R China
3.Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou, Guangdong, Peoples R China
4.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
5.Univ Sci & Technol China, Nano Sci & Technol Inst, Suzhou 215123, Peoples R China
推荐引用方式
GB/T 7714
Zhao, Kun,Chen, Jing,Li, Haibin,et al. Effects of Co-substitution on the reactivity of double perovskite oxides LaSrFe2-xCoxO6 for the chemical-looping steam methane reforming[J]. JOURNAL OF THE ENERGY INSTITUTE,2019,92(3):594-603.
APA Zhao, Kun,Chen, Jing,Li, Haibin,Zheng, Anqing,&He, Fang.(2019).Effects of Co-substitution on the reactivity of double perovskite oxides LaSrFe2-xCoxO6 for the chemical-looping steam methane reforming.JOURNAL OF THE ENERGY INSTITUTE,92(3),594-603.
MLA Zhao, Kun,et al."Effects of Co-substitution on the reactivity of double perovskite oxides LaSrFe2-xCoxO6 for the chemical-looping steam methane reforming".JOURNAL OF THE ENERGY INSTITUTE 92.3(2019):594-603.
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