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多层核壳结构Fe@Al-Ti载氧体化学链制氢性能研究

蔡志阳 张俊贤 汪欣 肖慧霞 高云飞 王亦飞

蔡志阳, 张俊贤, 汪欣, 肖慧霞, 高云飞, 王亦飞. 多层核壳结构Fe@Al-Ti载氧体化学链制氢性能研究[J]. 燃料化学学报(中英文), 2024, 52(3): 353-361. doi: 10.19906/j.cnki.JFCT.2023072
引用本文: 蔡志阳, 张俊贤, 汪欣, 肖慧霞, 高云飞, 王亦飞. 多层核壳结构Fe@Al-Ti载氧体化学链制氢性能研究[J]. 燃料化学学报(中英文), 2024, 52(3): 353-361. doi: 10.19906/j.cnki.JFCT.2023072
CAI Zhiyang, ZHANG Junxian, WANG Xin, XIAO Huixia, GAO Yunfei, WANG Yifei. Chemical looping hydrogen generation with multi-layer core-shell oxygen carrier of Fe@Al-Ti[J]. Journal of Fuel Chemistry and Technology, 2024, 52(3): 353-361. doi: 10.19906/j.cnki.JFCT.2023072
Citation: CAI Zhiyang, ZHANG Junxian, WANG Xin, XIAO Huixia, GAO Yunfei, WANG Yifei. Chemical looping hydrogen generation with multi-layer core-shell oxygen carrier of Fe@Al-Ti[J]. Journal of Fuel Chemistry and Technology, 2024, 52(3): 353-361. doi: 10.19906/j.cnki.JFCT.2023072

多层核壳结构Fe@Al-Ti载氧体化学链制氢性能研究

doi: 10.19906/j.cnki.JFCT.2023072
详细信息
    通讯作者:

    Tel:021-64252522, E-mail: wangyf@ecust.edu.cn

  • 中图分类号: TQ116.2

Chemical looping hydrogen generation with multi-layer core-shell oxygen carrier of Fe@Al-Ti

  • 摘要: Fe-Al-Ti载氧体在化学链制氢工艺中具有良好的循环稳定性和抗积炭性能,但反应形成FeAl2O4会降低抗烧结性能和氢气产率。为抑制FeAl2O4的生成并进一步提升载氧体反应性能,本研究采用自组装模板燃烧法制备多层核壳结构载氧体,以TiO2为介层阻隔Fe2O3与Al2O3,形成多层核壳Fe@Al-Ti载氧体,在固定床上进行化学链制氢循环,评价多层核壳结构对反应性能的影响。结果表明,Fe@Al-Ti载氧体的介层有效阻隔Fe2O3与Al2O3的接触,抑制了FeAl2O4形成,抗烧结性能得到进一步提升。Fe@Al-Ti载氧体在化学链制氢循环实验中无明显积炭和团聚现象,制氢能力随循环次数逐渐增加,循环稳定性较好;尤其物质的量比Al∶Ti=3.5∶1的核壳载氧体的碳转化率、制氢率和储氧量最高,分别为57.4%、75.0%和6.01 mmol/g,比非核壳Fe-Al-Ti载氧体分别增加28.4%、30.0%、26.9%。
  • FIG. 3014.  FIG. 3014.

    FIG. 3014.  FIG. 3014.

    图  1  Al2O3-TiO2聚合体TEM显微照片

    Figure  1  TEM micrographs of the Al2O3-TiO2 agglomerates

    图  2  化学链制氢固定床装置示意图

    Figure  2  Schematic diagram of fixed bed for chemical looping hydrogen generation

    图  3  不同载氧体20次循环下碳转化率变化

    Figure  3  Carbon conversion rate of different oxygen carriers under 20 cycles

    图  4  不同载氧体20次循环积炭率

    Figure  4  Carbon deposition rate of different oxygen carriers in 20 cycles

    图  5  不同载氧体20次循环下H2产量

    Figure  5  Hydrogen yield of different oxygen carriers under 20 cycles

    图  6  不同载氧体20次循环下储氧量变化

    Figure  6  Oxygen Storage Capacity of different oxygen carriers under 20 cycles

    图  7  不同载氧体单次循环中H2产率随时间变化趋势(第3、10、17次循环)

    Figure  7  H2 yield of different oxygen carriers in a single cycle (Cycle No.3, 10 and 17)

    图  8  载氧体循环前后平均粒径

    Figure  8  The average grain size of oxygen carriers before and after cycles

    图  9  载氧体化学链制氢循环前后SEM照片

    Figure  9  SEM images of oxygen carriers before and after cycles

    图  10  载氧体化学链制氢循环前后XRD谱图

    Figure  10  XRD patterns of oxygen carriers before and after cycles

    表  1  载氧体制备原料及制备方法

    Table  1  Materials and methods of oxygen carriers prepared in this work

    SamplePreparation methodMaterials/g
    Al2O3TiO2Fe(NO3)3·9H2OCO(NH2)2
    SATC(3.5∶1)SATC7.002.0068.1823.25
    SATC(2∶1)SATC6.003.0068.1823.25
    IMImpregnation7.002.0068.18
    Sol-gelSol-gel9.0068.18
    下载: 导出CSV

    表  2  化学链制氢实验循环工况

    Table  2  Experimental procedure in a cycle

    No.Experimental stageTime/minGas flow rate/(L·min−1)
    1CO reduction20CO∶0.30 N2∶1.50
    2nitrogen blowing8N2∶1.50
    3steam oxidization4N2∶1.50 H2O(l)∶0.45
    4nitrogen blowing8N2∶1.50
    5air oxidization10O2∶0.30 N2∶1.50
    6nitrogen blowing8N2∶1.50
    下载: 导出CSV

    表  3  载氧体XRD物相及晶体尺寸

    Table  3  XRD phase and crystallite of oxygen carrier

    Crystal formCrystallite/Å
    freshafter 10 cyclesafter 20 cycles
    SATC(3.5∶1)Fe2TiO5365.5
    FeAl2O4
    SATC(2∶1)Fe2TiO5364.7364.7
    FeAl2O4406.5
    IMFe2TiO5370.0366.6363.8
    FeAl2O4437.4496.5
    下载: 导出CSV
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出版历程
  • 收稿日期:  2023-06-20
  • 修回日期:  2023-08-05
  • 录用日期:  2023-08-28
  • 网络出版日期:  2023-09-28
  • 刊出日期:  2024-03-08

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