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CO在不同氧缺陷Cu1/CeO2(110)表面的吸附:DFT + U

张佳松 王辉 王宁 孙健伟 杨建成

张佳松, 王辉, 王宁, 孙健伟, 杨建成. CO在不同氧缺陷Cu1/CeO2(110)表面的吸附:DFT + U[J]. 燃料化学学报(中英文), 2022, 50(3): 326-336. doi: 10.1016/S1872-5813(21)60149-4
引用本文: 张佳松, 王辉, 王宁, 孙健伟, 杨建成. CO在不同氧缺陷Cu1/CeO2(110)表面的吸附:DFT + U[J]. 燃料化学学报(中英文), 2022, 50(3): 326-336. doi: 10.1016/S1872-5813(21)60149-4
ZHANG Jia-song, WANG Hui, WANG Ning, SUN Jian-wei, YANG Jian-cheng. Adsorption of CO on Cu1/CeO2(110) surface with different oxygen defects: DFT + U[J]. Journal of Fuel Chemistry and Technology, 2022, 50(3): 326-336. doi: 10.1016/S1872-5813(21)60149-4
Citation: ZHANG Jia-song, WANG Hui, WANG Ning, SUN Jian-wei, YANG Jian-cheng. Adsorption of CO on Cu1/CeO2(110) surface with different oxygen defects: DFT + U[J]. Journal of Fuel Chemistry and Technology, 2022, 50(3): 326-336. doi: 10.1016/S1872-5813(21)60149-4

CO在不同氧缺陷Cu1/CeO2(110)表面的吸附:DFT + U

doi: 10.1016/S1872-5813(21)60149-4
基金项目: 国家自然科学基金(51676058)资助
详细信息
    作者简介:

    张佳松:18222158863@163.com

    通讯作者:

    E-mail: wanghui_hb@hit.edu.cn

  • 中图分类号: TQ534.9

Adsorption of CO on Cu1/CeO2(110) surface with different oxygen defects: DFT + U

Funds: The project was supported by the National Natural Science Foundation of China (51676058)
  • 摘要: 本研究基于量子化学的密度泛函理论(DFT)研究了CO在理想和氧缺陷Cu1/CeO2(110)表面上的吸附,并且对CO分子在催化剂表面不同位点的吸附特性进行了计算和分析。结果表明,Cu掺杂可以显著提高CO在催化剂表面的吸附性能,顶位是CO最稳定的吸附位,CO在空穴位上的吸附能力很弱。与理想表面相比,线性缺陷的构造可以进一步提高CO在催化剂表面的吸附性能。对吸附构型PDOS的分析表明,大量的轨道杂化是CO在Cu1/CeO2(110)表面吸附性能较强的原因。
  • FIG. 1387.  FIG. 1387.

    FIG. 1387.  FIG. 1387.

    图  1  CO在CeO2(110)表面的吸附

    Figure  1  Adsorption of CO on CeO2(110) surface

    (a): Ce atom top position (C-down); (b): Ce atom top position (O-down); (c): O atom top position (C-down); (d): O atom top position (O-down); (e): bridge site (C-down); (f): bridge site (O-down); (g): empty acupoints (C-down); (h): empty acupoints (O-down)

    图  2  铜掺杂结构示意图

    Figure  2  Copper doped structure

    (a): front view; (b): top view (pink: Cu atom; red: O atom; white: Ce atom)

    图  3  CO在无缺陷表面的吸附(C-down)

    Figure  3  Adsorption of CO on defect-free surface (C-down)

    (A: top site; B: bridge site; C: empty acupoints; G-O: Geometry Optimization; the same below)

    图  4  CO在无缺陷表面的吸附(O-down)

    Figure  4  Adsorption of CO on defect-free surface (O-down)

    图  5  CeO2(110)表面不同氧缺陷类型

    Figure  5  Different oxygen defect types on CeO2(110) surface

    (a): single oxygen defect; (b): linear oxygen defect; (c): triangular oxygen defect

    图  6  CO在氧缺陷表面的吸附

    Figure  6  Adsorption of CO on oxygen defect surface

    (a): adsorption of CO on single oxygen defect surface; (b): adsorption of CO on linear oxygen defect surface; (c): adsorption of CO on triangular oxygen defect surface

    图  7  CO吸附在无缺陷表面上时C与Cu的PDOS

    Figure  7  PDOS of C and Cu with CO adsorbed on defect free surface

    图  8  CO吸附在单个氧原子缺陷表面上时C与Cu的PDOS

    Figure  8  PDOS of C and Cu when CO adsorbed on the surface of single oxygen atom defect

    图  9  CO吸附在线性氧缺陷表面上时C与Cu的PDOS

    Figure  9  PDOS of C and Cu when CO adsorbs on linear oxygen defect surface

    图  10  CO吸附在三角形氧缺陷表面上时C与Cu的PDOS

    Figure  10  PDOS of C and Cu when CO adsorbs on triangular oxygen defect surface

    表  1  无缺陷表面吸附数据(C-down)

    Table  1  Surface adsorption data without defects (C-down)

    Adsorption configurationConfigurationsRCO-surface/nmDC-Cu/nmQCO/e
    Defect-free surface1A0.1160.1790.173
    1B0.1160.1780.173
    1C0.1140.3350.050
    下载: 导出CSV

    表  2  无缺陷表面吸附数据(O-down)

    Table  2  Surface adsorption data without defects (O-down)

    Adsorption configurationConfigurationsRCO-surface/nmDC-Cu/nmQCO/e
    Defect-free surface1A*0.1140.307−0.003
    1B*0.1140.316−0.002
    1C*0.1140.3760.009
    下载: 导出CSV

    表  3  不同缺陷表面吸附数据

    Table  3  Surface adsorption data of different defects

    Adsorption configurationConfigurationsRCO-surface/nmDC-Cu/nmQCO/e
    Single oxygen defect surface2A0.1160.1780.172
    2B0.1160.1780.174
    2C0.1140.3370.033
    Linear oxygen defect surface3A0.1170.1790.057
    3B0.1190.1790.099
    3C0.1280.394−0.718
    Triangular oxygen defect surface4A0.1190.1800.144
    4B0.1190.1800.141
    4C0.1170.391−0.080
    下载: 导出CSV
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  • 收稿日期:  2021-07-06
  • 修回日期:  2021-08-28
  • 网络出版日期:  2021-08-25
  • 刊出日期:  2022-03-28

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