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Ni/CeO2催化剂的金属-载体界面调控及其低温化学链甲烷干重整性能研究

李睿杰 章菊萍 史健 李孔斋 刘慧利 祝星

李睿杰, 章菊萍, 史健, 李孔斋, 刘慧利, 祝星. Ni/CeO2催化剂的金属-载体界面调控及其低温化学链甲烷干重整性能研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(22)60032-X
引用本文: 李睿杰, 章菊萍, 史健, 李孔斋, 刘慧利, 祝星. Ni/CeO2催化剂的金属-载体界面调控及其低温化学链甲烷干重整性能研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(22)60032-X
LI Rui-jie, ZHANG Ju-ping, SHI Jian, LI Kong-zhai, LIU Hui-li, ZHU Xing. Metal-support interface regulation of Ni/CeO2 catalyst and low temperature chemical looping dry reforming of methane performance[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(22)60032-X
Citation: LI Rui-jie, ZHANG Ju-ping, SHI Jian, LI Kong-zhai, LIU Hui-li, ZHU Xing. Metal-support interface regulation of Ni/CeO2 catalyst and low temperature chemical looping dry reforming of methane performance[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(22)60032-X

Ni/CeO2催化剂的金属-载体界面调控及其低温化学链甲烷干重整性能研究

doi: 10.1016/S1872-5813(22)60032-X
基金项目: 国家自然科学基金(52066007),云南省基础研究计划项目(202101AT070076)和云南省高层次人才培养支持计划资助
详细信息
    作者简介:

    李睿杰(1998-),男,江苏扬州人,昆明理工大学硕士生

    刘慧利,E-mail:lhlqwer@163.com

    祝星,Email: zhuxing2010@hotmail.com

    通讯作者:

    Email: lhlqwer@163.com

    zhuxing2010@hotmail.com;Tel.: +86-13987129614

  • 中图分类号: O643;0614

Metal-support interface regulation of Ni/CeO2 catalyst and low temperature chemical looping dry reforming of methane performance

Funds: Supported by the National Science Foundation of China (52066007) and the Basic research Program of Yunnan Province and the High-level Talents Training Support Program of Yunnan Provinc (202101AT070076)
  • 摘要: 本研究合成了四种CeO2形貌的Ni/CeO2催化剂(纳米棒、纳米立方体、纳米八面体和纳米多面体),并探讨了催化剂低温化学链甲烷干重整反应的结构依赖性。 材料表征表明,Ni物种高度分散在CeO2载体表面,部分Ni离子进入CeO2晶格,从而引起氧空位的增加。化学链干重整性能测试结果表明,棒状结构Ni/CeO2催化剂表现出最高的还原性,具有最多氧空位和最高储氧能力。多面体状Ni/CeO2催化剂的结构为形状不规则的约10.3 nm的CeO2纳米单晶,具有较高的比表面积和较高的还原性,表现出低温甲烷反应活性,在550 ℃低温化学链甲烷干重整中显示最高的氧化还原活性和循环稳定性。本研究为设计高效的金属/CeO2催化剂提供了一种新策略,有望促进铈基催化剂在化学链技术中应用。
  • 图  1  CeO2水热处理的形貌相图

    Figure  1  Morphological phase diagram of CeO2 after hydrothermal treatment[31]

    图  2  (a)CeO2、(b)NiO/CeO2和(c、d)Ni/CeO2的XRD谱图

    Figure  2  XRD patterns of (a) CeO2, (b) NiO/CeO2, and (c, d) Ni/CeO2

    图  3  (a)Ni/CeO2-R、(b)Ni/CeO2-C、(c)Ni/CeO2-P的N2吸附-解吸等温线和孔径分布(插图)

    Figure  3  N2 adsorption-desorption isotherms and pore size distribution (inset) of (a) Ni/CeO2-R, (b) Ni/CeO2-C, (c) Ni/CeO2-P

    图  4  新鲜制备的CeO2的SEM、TEM和HRTEM图像

    Figure  4  SEM, TEM and HRTEM images of as-obtained CeO2 (a, b, c) CeO2-R, (d, e, f) CeO2-C, (g, h, i) CeO2-P and (j, k, l) CeO2-O

    图  5  Ni/CeO2的TEM和HRTEM图像

    Figure  5  TEM and HRTEM images of Ni/CeO2

    (a, d) Ni/CeO2-R, (b, e) Ni/CeO2-C and (c, f) Ni/CeO2-P

    图  6  (a)CeO2样品,(b)Ni/CeO2样品的拉曼光谱谱图

    Figure  6  Raman spectra of (a) CeO2 samples (b) Ni/CeO2 samples

    图  7  CH4的温度程序反应(CH4-TPR)曲线:(a)Ni/CeO2-R,(b)Ni/CeO2-C,(c)Ni/CeO2-P;(d)Ni/CeO2:(e)CH4-TPR过程中生成物形成的起始温度

    Figure  7  Temperature-programmed reaction of CH4 (CH4-TPR) profiles over (a)Ni/CeO2-R, (b) Ni/CeO2-C, (c) Ni/CeO2-P; (d) Ni/CeO2,( e)starting temperature of products formation during the CH4-TPR

    图  8  (a)Ni/CeO2-R、(b)Ni/CeO2-C、(c)Ni/CeO2-P和(d)Ni/CeO2的氧化还原反应产生的气体

    Figure  8  Gaseous from the redox reactions over (a) Ni/CeO2-R, (b) Ni/CeO2-C and (c) Ni/CeO2-P和(d)Ni/CeO2

    图  9  (a)在不同的Ni/CeO2氧化还原催化剂上,甲烷氧化步骤中CH4的转化率、CO的选择性和CO2的转化率;(b)甲烷氧化步骤中H2、CO和CO2的产率和CO2分裂步骤中CO的产率。

    Figure  9  (a) CH4 conversion, CO selectivity and CO2 conversion in methane step over different Ni/CeO2 redox catalyst; (b)Yields of H2, CO and CO2 in methane oxidation step and CO yield in CO2 splitting step

    图  10  用于CLDRM的Ni/CeO2氧化还原催化剂的氧化还原稳定性:(a)在550 ℃下,三种Ni/CeO2氧化还原催化剂在连续氧化还原循环中的CH4转化和CO2转化;(b) 在Ni/CeO2-P氧化还原催化剂上,甲烷氧化步骤中H2、CO和CO2的产率以及CO2分裂步骤中CO的产率

    Figure  10  Redox stability of Ni/CeO2 redox catalysts for CL-DRM (a) CH4 conversion and CO2 conversion in successive redox cycles over three Ni/CeO2 redox catalyst at 550 ℃. (b) Yield of H2, CO and CO2 in methane oxidation step and CO yield in CO2 splitting step over Ni/CeO2-P redox catalyst at 550 ℃ during the 50 redox cycles.

    图  11  反应后Ni/CeO2样品的XRD谱图

    Figure  11  XRD patterns of spent Ni/CeO2 samples.

    图  12  Ni/CeO2-P的TEM图

    Figure  12  TEM images of spent Ni/CeO2-P

    表  1  CeO2纳米结构水热合成条件

    Table  1  Hydrothermal synthesis conditions of CeO2 nanostructures

    Supports${{C} }_{ {\rm{NaOH/Na_3PO_4} } }$
    (mol·L−1)
    t/℃t/hStructureShape
    CeO2-R610024cubicrods
    CeO2-C718024cubiccubes
    CeO2-P0.510024cubicparticles
    CeO2-O0.000317010cubicoctahedra
    Note: Synthesized under [Ce3+] = 0.4 mol/L
    下载: 导出CSV

    表  2  Ni/CeO2样品中CeO2的晶格参数(a0)、结晶尺寸和微应变(ε)

    Table  2  The lattice parameter (a0), crystalline size,and the microstrain (ε) of ceria in Ni/CeO2 samples.

    Sampled(111)-spacing/nmLattice parameter/nmCeO2 crystalline size/nmε/%
    (111)(220)(311)avg.
    Ni/CeO2-R0.311220.54113411.211.211.411.40.084
    Ni/CeO2-C0.311860.541058 > 100 > 100 > 100319.70.020
    Ni/CeO2-P0.312070.54060910.210.510.710.30.027
    Ni/CeO2-O0.310440.53957560.153.951.355.10.058
    下载: 导出CSV

    表  3  煅烧后的Ni/CeO2催化剂的织构性能

    Table  3  Textural property of calcined Ni/CeO2 catalysts

    SampleSBET/(m2·g−1)Pore
    volume/(cm3·g−1)
    Average pore
    size/nm
    Ni/CeO2-R57.880.2661.0
    Ni/CeO2-C7.930.0219.2
    Ni/CeO2-P60.910.1747.4
    Ni/CeO2-O12.010.0324.5
    下载: 导出CSV
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  • 收稿日期:  2022-03-16
  • 录用日期:  2022-04-24
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