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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Theoretical Study on the Decomposition of N_2O over Alkaline Earth Metal-Oxides: MgO-BaO
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Theoretical Study on the Decomposition of N_2O over Alkaline Earth Metal-Oxides: MgO-BaO

机译：N_2O在碱土金属氧化物MgO-BaO上分解的理论研究

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摘要

The decomposition of N_2O through oxygen abstraction and surface peroxide ion formation is studied over the whole sequence, MgO-BaO, of alkaline-earth rock-salt metal oxides. The initial barrier to abstraction follows the expectations (MgO > CaO > SrO > BaO) of O~(2-) chemistry. Good agreement with experiment is obtained for MgO and CaO, but for BaO the discrepancy is large. Consideration of both the Langmuir-Hinshelwood and the Elay-Rideal mechanisms suggests that for MgO the surface is regenerated already at low peroxide ion coverage through diffusion and recombination. For CaO, diffusion is hindered and recombination probably occurs only at higher peroxide ion coverage obtained through deposition of oxygen. SrO and BaO allow neither diffusion over the surface nor recombination of oxygen from two surface peroxide ions. Instead, the Elay-Rideal mechanism becomes active with activation energy at high coverage in good agreement with the experimental for BaO.
机译：在碱土岩盐金属氧化物的整个过程MgO-BaO上，研究了N_2O通过吸氧分解和形成表面过氧化物离子而分解的过程。最初的抽象障碍遵循对O〜（2-）化学的期望（MgO> CaO> SrO> BaO）。 MgO和CaO与实验结果吻合良好，但BaO的差异较大。对兰格缪尔-欣沙尔伍德和Elay-Rideal机理的综合考虑表明，对于MgO，表面已经通过扩散和重组以低过氧化物离子覆盖率进行了再生。对于CaO，扩散受到阻碍，并且重组可能仅在通过氧气沉积获得的更高的过氧化物离子覆盖率下发生。 SrO和BaO既不允许在表面上扩散，也不允许来自两个表面过氧化物离子的氧复合。取而代之的是，Elay-Rideal机制在高覆盖率下具有活化能，并且与BaO实验非常吻合。

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