取决于场的电极 - 化学酸盐结合:对振动的敏感性和结合能量与表面协调的性质有关
Sally A Wasileski1, Marc T M Koper, Michael J Weaver
1Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, USA.
Journal of the American Chemical Society
|March 14, 2002
概括
外部电场揭示了不同吸附物如何与表面结合. 这项研究根据电荷偏振和振动频率对表面结合进行了分类,有助于电化学系统设计.
科学领域:
- 表面科学是一门学科.
- 计算化学计算化学
- 电化学 电化学 电化学
背景情况:
- 对于电化学系统来说,了解金属吸附剂相互作用至关重要.
- 振动的斯塔克效应量化了外部场如何改变振动频率.
- 对表面协调的敏感性会影响结合的能量和频率.
研究的目的:
- 为了研究外部电场对化学吸附剂结合的影响.
- 为了确定绑定能量和振动频率对表面协调的灵敏度.
- 根据其电子和粘合特性对吸附剂进行分类.
主要方法:
- 密度函数理论 (DFT) 在白金集群模型上的计算.
- 原子和分子化学酸盐 (Cl,I,O,N,Na,NH3,CO) 的模拟.
- 对电场依赖的静态 (μS) 和动态 (μD) 双极电流的分析.
主要成果:
- 束能量场的斜率取决于电荷极化方向 (μS).
- 振动Stark调主要由动态二极极矩 (μD) 控制.
- 基于μS和μD的行为出现了一般的吸附物分类,区分离子和原始对应键.
结论:
- 这项研究清楚地区分了使用振动Stark调和结合能量场斜率的不同表面粘合类型.
- 电子阴性吸附体显示负μS和μD,而电阳性吸附体显示相反.
- 附带的附加剂 (NH3,CO) 呈现μS和μD与相反的标志由于减少轨道重叠.
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