氯化亚铜在活性炭载体表面单层分散的密度泛函理论计算

Density Functional Theory Calculations of Cuprous Chloride Monolayer Supported on Activated Carbon

应用量子化学计算方法研究了活性炭载体表面CuCl活性组分的单层分散行为 .以C16H10 ,C13 H9和C12 H12 原子簇模型模拟活性炭表面 ,用密度泛函理论中的B3LYP方法计算得到了CuCl在活性炭表面分散的活性位、稳定构型、相互作用能以及单层分散阈值 .结果表明 ,CuCl以铜端垂直附着在活性炭表面的顶位和桥位上 ,相互作用能为 76 84～ 80 79kJ/mol,单层分散阈值为 0 4 71g/ g.而XRD测得的单层分散阈值为 0 4 6 7g/ g,与量子化学计算的结果一致 ;按照密置单层模型计算得出的单层分散阈值为 0 94 1g/g ,远大于实验测定结果 .因此 ,应用量子化学计算方法可以得到活性炭表面活性组分单层分散的丰富信息 ,并能确定活性组分的单层分散阈值 .

The density functional theory (DFT) was applied to investigate the monolayer dispersion behavior of cuprous chloride on activated carbon surface. The calculation was performed by B3LYP approach using LanL2DZ basis set for Cu and Cl atoms, and 6-31G * basis set for C and H atoms. The C 16 H 10 , C 13 H 9 and C 12 H 12 clusters were used to model the active sites of bridge, top and hole on activated carbon. The results showed that CuCl preferred to disperse on the surface top site or bridge site of activated carbon. The interaction energy was from 76 84 to 80 79 kJ/mol . The dispersion threshold of CuCl on activated carbon was 0 471 g/g , which is in agreement with the value measured by XRD method (0 467 g/g ). While the dispersion threshold calculated with the close-packed model was 0 941 g/g . Using DFT method can get not only abundant adsorption information about CuCl on activated carbon, but also its dispersion threshold.