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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >First-Principles Study of the Interaction between NO and Large Carbonaceous Clusters Modeling the Soot Surface
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First-Principles Study of the Interaction between NO and Large Carbonaceous Clusters Modeling the Soot Surface

机译：NO和模拟烟尘表面的大型碳质团簇相互作用的第一性原理研究

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First-principles calculations are performed to characterize the NO adsorption on large carbonaceous clusters modeling the surface of soot. Adsorption on the face and on the edges of perfect and defective clusters is considered in the calculations. It is shown that the first situation corresponds to physisorption and requires taking into account long-range dispersion interactions in the calculations. In contrast, interaction of NO with the unsaturated edge of a defective cluster leads preferentially to a C?N rather than to a C?O chemical binding. This indicates that soot may be an efficient sink for NO in the troposphere only if it contains a high number of unsaturated carbon atoms. From a more fundamental point of view, this study also clearly evidences that quantum calculations have to be carefully conducted when considering the interaction between radical species and carbonaceous surfaces. Problems encountered with the choice of the functional used in density functional theory approaches as well as with the size of the basis set, spin multiplicity, and spin contamination have to be systematically addressed before any relevant conclusion can be drawn.
机译：进行第一性原理计算以表征在模拟烟灰表面的大型碳质团簇上的NO吸附特性。计算中考虑了完美和有缺陷簇的表面和边缘的吸附。结果表明，第一种情况对应于物理吸附，并且需要在计算中考虑远程色散相互作用。相反，NO与缺陷簇的不饱和边缘的相互作用优先导致C 2 N而不是C 2 O的化学键合。这表明，仅当烟灰中含有大量不饱和碳原子时，它才是对流层NO的有效吸收剂。从更基本的角度来看，这项研究还清楚地表明，在考虑自由基物种与碳质表面之间的相互作用时，必须谨慎进行量子计算。在得出任何相关结论之前，必须系统地解决在密度泛函理论方法中使用的泛函的选择以及基集的大小，自旋多重性和自旋污染所遇到的问题。

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