Adsorption of CO on Cu1/CeO2(110) surface with different oxygen defects: DFT + U
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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。Abstract: Adsorption of CO on ideal and oxygen deficient Cu1/CeO2(110) surfaces was studied by density functional theory (DFT), and the adsorption characteristics of CO molecules at different sites on the modelled catalyst surface were calculated and analyzed. The results show that Cu-doping can significantly improve the adsorption performance of CO on the catalyst surface. The top position is the most stable adsorption site of CO, but the adsorption of CO on empty acupoints is very weak. Compared with the ideal surface, the linear defect structure can promote the adsorption of CO on the catalyst surface. The PDOS analysis of adsorption configuration shows that a large number of orbital hybridization may be the reason for the strong adsorption performance of CO on Cu1/CeO2(110) surface.
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Key words:
- adsorption /
- CO-SCR /
- oxygen vacancy /
- density functional theory /
- Cu doped
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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)
表 1 无缺陷表面吸附数据(C-down)
Table 1 Surface adsorption data without defects (C-down)
Adsorption configuration Configurations RCO-surface/nm DC-Cu/nm QCO/e Defect-free surface 1A 0.116 0.179 0.173 1B 0.116 0.178 0.173 1C 0.114 0.335 0.050 表 2 无缺陷表面吸附数据(O-down)
Table 2 Surface adsorption data without defects (O-down)
Adsorption configuration Configurations RCO-surface/nm DC-Cu/nm QCO/e Defect-free surface 1A* 0.114 0.307 −0.003 1B* 0.114 0.316 −0.002 1C* 0.114 0.376 0.009 表 3 不同缺陷表面吸附数据
Table 3 Surface adsorption data of different defects
Adsorption configuration Configurations RCO-surface/nm DC-Cu/nm QCO/e Single oxygen defect surface 2A 0.116 0.178 0.172 2B 0.116 0.178 0.174 2C 0.114 0.337 0.033 Linear oxygen defect surface 3A 0.117 0.179 0.057 3B 0.119 0.179 0.099 3C 0.128 0.394 −0.718 Triangular oxygen defect surface 4A 0.119 0.180 0.144 4B 0.119 0.180 0.141 4C 0.117 0.391 −0.080 -
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