化工学报2024,Vol.75Issue(12) :4532-4546.DOI:10.11949/0438-1157.20240633

Sr改性LaFeO3用于甲烷化学链重整的还原性能与动力学研究

Study on reduction performance and kinetics of Sr-modified LaFeO3 for methane chemical looping reforming

马浩天 荆体瑞 刘程程 玉散·吐拉甫 张喆 王一迪 王庆宏 陈春茂 徐春明
化工学报2024,Vol.75Issue(12) :4532-4546.DOI:10.11949/0438-1157.20240633

Sr改性LaFeO3用于甲烷化学链重整的还原性能与动力学研究

Study on reduction performance and kinetics of Sr-modified LaFeO3 for methane chemical looping reforming

马浩天 1荆体瑞 1刘程程 1玉散·吐拉甫 2张喆 2王一迪 1王庆宏 1陈春茂 1徐春明1
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作者信息

  • 1. 中国石油大学(北京)化学工程与环境学院,重质油全国重点实验室,北京 102249
  • 2. 清华大学环境学院,北京 100084
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摘要

甲烷化学链重整是新型低碳的制氢技术,载氧体还原特性是决定化学链重整制氢产率的关键因素.重点探讨了不同比例Sr掺杂对LaFeO3还原特性的影响,通过表征FeO6八面体畸变和表面氧形态分析了Sr掺杂对氧空位浓度、晶格氧传递的作用.La0.8Sr0.2FeO3具有明显的FeO6八面体畸变,表现出最低的晶格氧还原温度750℃,恒温还原中La0.8Sr0.2FeO3的最大失重量为LaFeO3的2~3倍.动力拟合计算发现La1-xSrxFeO3的还原过程均受成核核增长模型控制,同时受自催化模型影响,4种载氧体中,La08Sr02FeO3表现出最低的表观活化能.La0.8Sr0.2FeO3在水蒸气氧化实验中的增重速率约为LaFeO3的4倍,并且在20周期循环后保持原有物相不变.La1-xSrFeO3化学链重整与多周期稳定性的研究为甲烷化学链重整制氢材料选择和工艺优化提供了技术与数据支撑.

Abstract

Chemical looping reforming of methane is a novel low-carbon hydrogen production technology.The reduction characteristics of the oxygen carrier are key factors determining the hydrogen production rate of chemical looping reforming.The effect of different proportions of Sr doping on the reduction characteristics of LaFeO3 was discussed in detail.By characterizing the octahedral distortion and surface oxygen morphology of FeO6,the effect of Sr doping on oxygen vacancy concentration and lattice oxygen transfer was analyzed.La08Sr02FeO3 exhibits significant FeO6 octahedral distortion,showing the lowest lattice oxygen reduction temperature at 750℃.In isothermal reduction,the maximum mass loss of La0.8Sr0.2FeO3 is 2-3 times that of LaFeO3.Kinetic fitting calculations revealed that the reduction process of La1-xSrxFeO3 is controlled by the nucleation and growth model,while also being influenced by the autocatalytic model.Among the four oxygen carriers,La0.8Sr0.2FeO3 exhibits the lowest apparent activation energy.The mass gain rate of La08Sr02FeO3 in steam oxidation experiments is about 4 times that of LaFeO3,and it maintains its original phase after 20 cycles.The study of La1-xSrxFeO3 in chemical looping reforming and multi-cycle stability provides technical and data support for the selection of materials and process optimization in methane chemical looping reforming for hydrogen production.

关键词

甲烷/制氢/动力学/化学链/钙钛矿

Key words

methane/hydrogen production/kinetics/chemical looping/perovskite

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出版年

2024
化工学报
中国化工学会 化学工业出版社

化工学报

CSTPCDCSCD北大核心
影响因子:1.26
ISSN:0438-1157
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