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污泥燃烧中H2O、SO2和CO2对PbO在CaO表面吸附的影响

史一林 何学富 王彦霖 乔晓磊 贾里 金燕

史一林, 何学富, 王彦霖, 乔晓磊, 贾里, 金燕. 污泥燃烧中H2O、SO2和CO2对PbO在CaO表面吸附的影响[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2023001
引用本文: 史一林, 何学富, 王彦霖, 乔晓磊, 贾里, 金燕. 污泥燃烧中H2O、SO2和CO2对PbO在CaO表面吸附的影响[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2023001
SHI Yi-lin, HE Xue-fu, WANG Yan-lin, QIAO Xiao-lei, JIA Li, JIN Yan. Effect of flue gas components on PbO adsorption in CaO surface during sewage sludge combustion[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2023001
Citation: SHI Yi-lin, HE Xue-fu, WANG Yan-lin, QIAO Xiao-lei, JIA Li, JIN Yan. Effect of flue gas components on PbO adsorption in CaO surface during sewage sludge combustion[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2023001

污泥燃烧中H2O、SO2和CO2对PbO在CaO表面吸附的影响

doi: 10.19906/j.cnki.JFCT.2023001
基金项目: 国家自然科学基金(U1910124)项目资助
详细信息
    通讯作者:

    E-mail: jinyan@tyut.edu.cn

  • 中图分类号: TQ534

Effect of flue gas components on PbO adsorption in CaO surface during sewage sludge combustion

Funds: The project was supported by the National Natural Science Foundation of China (U1910124)
  • 摘要: 采用密度泛函理论研究了污泥燃烧过程中烟气组分对PbO在CaO(001)表面吸附的影响。计算结果表明,CaO(001)表面的 O顶位是PbO分子、H2O分子、SO2分子和CO2分子吸附的活性位点。H2O分子、SO2分子和CO2分子的存在分别使PbO分子在CaO(001)表面的吸附能较洁净表面增大了71.42、19.589和46.431kJ/mol。H2O分子在吸附过程中形成的OH基团和局部Ca(OH)2表面结构有利于PbO分子的吸附。SO2分子中的OS原子和CaO(001)表面的Osurf原子的态密度轨道均与Pb原子轨道产生重叠,使得PbO分子在表面的吸附更加稳定。CO2分子预吸附在CaO(001)表面形成的CO3基团对PbO分子存在强吸附作用,使得PbO分子更稳定的吸附在CaO(001)表面。
  • 图  1  CaO(001)周期性板块模型

    Figure  1  CaO (001) periodic plate model

    图  2  PbO在CaO(001)表面优化前后的吸附结构

    Figure  2  A dsorption structure of PbO before and after optimization on CaO(001) surface

    图  3  PbO分子在CaO(001)表面吸附的电子密度图和PDOS

    Figure  3  Electron density map and PDOS of PbO molecules on the surface of CaO(001)

    图  4  H2O在CaO(001)表面优化前后的吸附结构

    Figure  4  A dsorption structure of H2O before and after optimization on the surface of CaO (001)

    图  5  H2O分子稳定吸附于CaO(001)表面的电子密度图和差分电荷密度图

    Figure  5  Electron density map and differential charge density map of H2O molecules stably adsorbed on the surface of CaO(001)

    图  6  SO2在CaO(001)表面优化前后的吸附结构

    Figure  6  A dsorption structure of SO2 before and after optimization on CaO(001) surface

    图  7  SO2分子稳定吸附于CaO(001)表面的电子密度图和差分电荷密度图

    Figure  7  Electron density map and differential charge density map of SO2 molecules stably adsorbed on the surface of CaO(001)

    图  8  CO2在CaO(001)表面优化前后的吸附结构

    Figure  8  A dsorption structure of CO2 before and after optimization on CaO(001) surface

    图  9  CO2分子稳定吸附于CaO(001)表面的电子密度图和差分电荷密度图

    Figure  9  Electron density map and differential charge density map of CO2 molecules stably adsorbed on the surface of CaO(001)

    图  10  H2O对PbO在CaO表面吸附的影响

    Figure  10  Effect of H2O on the adsorption of PbO on CaO surface

    图  11  PbO分子在H2O + CaO(001)表面吸附后的电子密度图

    Figure  11  Electron density diagram of PbO molecules after adsorption on the surface of H2O + CaO(001)

    图  12  SO2对PbO在CaO表面吸附的影响

    Figure  12  Effect of SO2 on the adsorption of PbO on CaO surface

    图  13  Pb、OS原子和Osurf原子的PDOS

    Figure  13  PDOS of Pb, OS atom and Osurf atom

    图  14  CO2对PbO在CaO表面吸附的影响

    Figure  14  Effect of CO2 on the adsorption of PbO on CaO surface

    图  15  Pb、Osurf原子和OC原子的PDOS

    Figure  15  PDOS of Pb, Osurf atom and OC atom

    表  1  结构和能量收敛标准

    Table  1  Structural and energy convergence criteria

    ParameterConvergence criteria
    SCF tolerance1.0 × 10−6 eV/atom
    energy tolerance1.0 × 10−5 eV/atom
    maximum displacement tolerance0.001 Å
    maximum force tolerance0.03 eV/Å
    下载: 导出CSV

    表  2  各分子优化后的键长和键角

    Table  2  Optimized bond length and bond angle for each molecule

    MoleculeKey ength /key angleOptimize value/(Å/°)Reference value/(Å/°)Relative error/%
    CaOCa-O4.9094.8052.164
    α=β=γ90900.000
    H2OH-O0.9780.961.875
    H-O-H103.741104.50.726
    SO2S-O1.4571.431.889
    O-S-O119.401119.50.083
    CO2C-O1.1731.1630.860
    O-C-O179.9901800.006
    PbOPb-O1.9461.921.354
    下载: 导出CSV

    表  3  PbO在CaO表面吸附的参数

    Table  3  Parameters of PbO after adsorption on CaO surface

    Adsorption structureEad/
    (kJ·mol−1
    Pb-O bond length/ÅPb-Osurf bond length/Åq(PbO)/e
    1-a−143.5402.0142.329−0.16
    1-b−126.8942.0132.291−0.19
    1-c−143.8672.0122.329−0.16
    1-d−143.6762.0112.330−0.16
    下载: 导出CSV

    表  4  H2O分子在CaO(001)表面吸附的参数

    Table  4  Parameters of H2O after adsorption on CaO surface

    Adsorption structureEad/
    (kJ·mol−1
    H−O bond length/Åq(H2O)/e
    2-a−74.2081.037−0.23
    2-b−85.2200.972−0.25
    2-c−91.4500.974−0.26
    2-d−28.3680.9800.01
    下载: 导出CSV

    表  5  SO2在CaO(001)表面吸附的参数

    Table  5  Parameters of SO2 after adsorption on CaO surface

    Adsorption structureEad/(kJ·mol−1S−Osurf distance/Åq(SO2)/e
    3-a−231.0853.088−0.08
    3-b−235.9523.232−0.16
    3-c−396.9921.697−0.28
    3-d−228.5413.615−0.06
    下载: 导出CSV

    表  6  CO2在CaO(001)表面吸附的参数

    Table  6  Parameters of CO2 after adsorption on CaO surface

    Adsorption structureEad/(kJ·mol−1C-Osurf distance/Åq(CO2)/e
    4-a−17.187−0.04
    4-b−122.7971.407−0.63
    4-c−122.8451.406−0.61
    4-d0.304−0.03
    下载: 导出CSV

    表  7  PbO在H2O/SO2/CO2 + CaO(001)表面吸附的吸附能、键参数和电荷转移

    Table  7  Adsorption energy, bond parameters and charge transfer of PbO adsorption on the surface of H2O/SO2/CO2 + CaO(001)

    Adsorption structureEad/
    (kJ·mol−1
    Pb-Osurf bond length/ÅPb-Osurf Population
    H2O−215.2872.5640.14
    SO2−163.4562.8360.11
    CO2−190.2982.4590.18
    下载: 导出CSV
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  • 收稿日期:  2022-11-24
  • 录用日期:  2022-12-27
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