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Ni/SSZ-13催化剂的CO2甲烷化反应性能研究

张锦川 杨应举 刘晶 华芷萱

张锦川, 杨应举, 刘晶, 华芷萱. Ni/SSZ-13催化剂的CO2甲烷化反应性能研究[J]. 燃料化学学报(中英文), 2021, 49(7): 960-966. doi: 10.19906/j.cnki.JFCT.2021041
引用本文: 张锦川, 杨应举, 刘晶, 华芷萱. Ni/SSZ-13催化剂的CO2甲烷化反应性能研究[J]. 燃料化学学报(中英文), 2021, 49(7): 960-966. doi: 10.19906/j.cnki.JFCT.2021041
ZHANG Jin-chuan, YANG Ying-ju, LIU Jing, HUA Zhi-xuan. Catalytic activity of Ni/SSZ-13 catalyst for CO2 methanation[J]. Journal of Fuel Chemistry and Technology, 2021, 49(7): 960-966. doi: 10.19906/j.cnki.JFCT.2021041
Citation: ZHANG Jin-chuan, YANG Ying-ju, LIU Jing, HUA Zhi-xuan. Catalytic activity of Ni/SSZ-13 catalyst for CO2 methanation[J]. Journal of Fuel Chemistry and Technology, 2021, 49(7): 960-966. doi: 10.19906/j.cnki.JFCT.2021041

Ni/SSZ-13催化剂的CO2甲烷化反应性能研究

doi: 10.19906/j.cnki.JFCT.2021041
基金项目: 中央高校基本科研业务费专项项目(2019KFYRCPY021)资助
详细信息
    作者简介:

    张锦川:z177965@163.com

    通讯作者:

    Tel: 027-87545526,E-mail: liujing27@mail.hust.edu.cn

  • 中图分类号: TK6

Catalytic activity of Ni/SSZ-13 catalyst for CO2 methanation

Funds: The project was supported by the Fundamental Research Funds for the Central Universities (2019KFYRCPY021)
  • 摘要: 采用浸渍法制备了Ni/SSZ-13催化剂,并研究了催化剂的CO2甲烷化反应性能。通过N2物理吸附-脱附、X射线衍射、扫描电子显微镜、透射电子显微镜、X射线光电子能谱等表征分析方法对催化剂的质构特性及物理化学性质进行了研究。结果表明,Ni/SSZ-13催化剂在250 ℃开始表现出CO2甲烷化催化活性;在450 ℃,Ni/SSZ-13表现出最佳的催化反应活性,CO2转化率和CH4选择性分别为70%和95%。SSZ-13载体表现出长方体结构,孔结构主要为微孔,并含有部分介孔,为镍物质的分散提供较大的比表面积。煅烧后的催化剂在500 ℃的还原过程中,NiO被H2还原成金属Ni,金属Ni是CO2甲烷化的主要活性组分。
  • FIG. 802.  FIG. 802.

    FIG. 802.  FIG. 802.

    图  1  不同反应温度条件下Ni/SSZ-13催化剂的CO2甲烷化反应性能

    Figure  1  Catalytic performance of SSZ-13 zeolite and Ni/SSZ-13 catalyst for CO2 methanation at different reaction temperatures

    (a): CO2 conversion; (b): CH4 and CO selectivity; (c): 24 h stability test

    图  2  SSZ-13沸石及Ni/SSZ-13催化剂的N2吸附-脱附等温曲线和孔径分布

    Figure  2  N2 adsorption-desorption isotherms and pore size distributions of SSZ-13 zeolite and Ni/SSZ-13 catalyst

    图  3  SSZ-13沸石和Ni/SSZ-13催化剂的XRD谱图

    Figure  3  XRD results of SSZ-13 zeolite and Ni/SSZ-13 catalyst

    图  4  SSZ-13载体和Ni/SSZ-13催化剂的SEM、TEM和EDS元素分布图

    Figure  4  SEM, TEM images and EDS elemental mapping of SSZ-13 zeolite and Ni/SSZ-13 catalyst

    (a): SEM image of SSZ-13 support; (b): SEM image of fresh Ni/SSZ-13 catalyst; (c): SEM image of spent Ni/SSZ-13 catalyst; (d): TEM image of fresh Ni/SSZ-13 catalyst; (e): TEM image of spent Ni/SSZ-13 catalyst; (f)−(h): EDS elemental mapping of SSZ-13 support; (i)−(l): EDS elemental mapping of fresh Ni/SSZ-13 catalyst

    图  5  还原后的Ni/SSZ-13催化剂表面Ni、O元素的XPS谱图

    Figure  5  XPS characterization spectra of Ni and O elements on the Ni/SSZ-13 catalyst surface after reduction (a): Ni 2p; (b): O 1s

    表  1  样品的比表面积及孔结构参数

    Table  1  The specific surface area and pore structure parameters of SSZ-13 zeolite and Ni/SSZ-13 catalyst

    SamplesSpecific surface
    area A/(m2·g−1)
    Micropore Area
    A/(m2·g−1)
    Pore volume
    v/(cm3·g−1)
    Micropore volume
    v/(cm3·g−1)
    Average pore
    size d/nm
    SSZ-13449.20337.690.280.173.61
    Ni/SSZ-13385.51284.030.240.144.53
    下载: 导出CSV

    表  2  Ni/SSZ-13催化剂的表面元素含量

    Table  2  Surface atom concentration of Ni/SSZ-13 catalyst

    C 1sO 1sAl 2pSi 2pNi 2p
    Peak BE284.77532.5874.79103.32854.94
    Atomic/%23.5251.431.1420.653.27
    下载: 导出CSV
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出版历程
  • 收稿日期:  2020-12-18
  • 修回日期:  2021-01-19
  • 网络出版日期:  2021-03-30
  • 刊出日期:  2021-07-15

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