Modulating lattice oxygen activity of Ca2Fe2O5 brownmillerite for the co-production of syngas and high purity hydrogen via chemical looping steam reforming of toluene

被引：65
作者：
Xu, Tingting [1 ,2 ,3 ,4 ]
Wang, Xun [1 ,7 ]
Zhao, Haibo [2 ]
Xiao, Bo [1 ]
Liu, Dong [3 ,4 ]
Liu, Wen [5 ,6 ]
机构：
[1] Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
[2] Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Wuhan 430074, Peoples R China
[3] Nanjing Univ Sci & Technol, Sch Energy & Power Engn, MIIT Key Lab Thermal Control Elect Equipment, Nanjing 210094, Peoples R China
[4] Nanjing Univ Sci & Technol, Sch Energy & Power Engn, Adv Combust Lab, Nanjing 210094, Peoples R China
[5] Nanyang Technol Univ, Sch Chem & Biomed Engn, 62 Nanyang Dr, Singapore 637459, Singapore
[6] Cambridge Ctr Adv Res & Educ, 1 CREATE Way, Singapore 138602, Singapore
[7] Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Luoyu Rd 1037, Wuhan, Peoples R China
来源：
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2023年 / 320卷
基金：
中国国家自然科学基金; 中国博士后科学基金; 新加坡国家研究基金会;
关键词：
Brownmillerite; Lattice oxygen activity; Chemical looping reforming; Syngas; Hydrogen; PERFORMANCE; CATALYSTS; CARRIERS; OXIDES;
D O I：
10.1016/j.apcatb.2022.122010
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
The chemical looping steam reforming (CLSR) of biomass tar enables the process intensification for the co -preparation of syngas and high purity hydrogen. The practical application of brownmillerite-structured Ca2Fe2O5 is hindered by activity-related issues such as low fuel conversion and oxygen transfer capacity. Here, the doping of heteroatoms, e.g. Ni induces structural changes to the brownmillerite lattice, transforming it from a Pnma phase to a Pcmn one, with increased distortion of the FeO6 octahedra. The structural changes lead to the upwards shifts of the O 2p band of oxygen carrier, and subsequently improved lattice oxygen activity as well as oxygen transfer capacity. The formation of oxygen vacancy is a rate determining step during CLSR, while the Ni-doped Ca2Fe2O5 reduces the energy of oxygen vacancy formation and energy barrier for lattice oxygen migration through the bulk. During CLSR, Ca2Ni0.25Fe1.75O5 lead to significant improvement in syngas pro-ductivity, hydrogen purity and fuel conversion.
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页数：11
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