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现场双光束巧合第二波生成作为在电化学接口的空间解析动态的探测器
Boguslaw Pozniak1, Daniel A Scherson
1Department of Chemistry, Case Western Reserve University, Cleveland, OH 44106-7078, USA.
Journal of the American Chemical Society
|November 13, 2004
概括
对 (Pt(111) 上的一氧化碳 (CO) 的空间分辨电氧化动态进行了监测. 结果显示,CO氧化发生在整个表面的不同时间,挑战了统一表面状态的假设.
科学领域:
- 表面科学是一门科学.
- 电化学 电化学 电化学
- 物理化学 物理化学
背景情况:
- 了解吸附物种在金属表面的电氧化对于催化是至关重要的.
- (111) 表面是研究二氧化碳氧化的一个模型系统.
- 之前的模型通常假定表面状态均.
研究的目的:
- 为了研究一氧化碳 (CO) 电氧化在Pt{111}表面的空间分辨力学.
- 为了确定CO扩散速率是否足以在氧化过程中保持均的表面状态.
- 将实验结果与来自平均场近似模型的预测进行比较.
主要方法:
- 在现场使用双光束巧合第二波生成 (SHG).
- 空间分辨率测量是在Pt{11}/CO和0.1M HClO4接口上进行的.
- 从30到870mV对比RHE的潜在步骤被应用.
主要成果:
- 通过SHG检测到的CO的完全电氧化发生在Pt(111) 表面的不同区域的不同时间.
- 在应用的电位范围中观察到氧化时间的这种空间异质性.
- 结果表明,在CO电氧化过程中,表面动态不均.
结论:
- 在电氧化过程中,吸附的二氧化碳的扩散速率并不总是足以使整个Pt111) 表面均化.
- 平均场近似,假设一个均的表面,可能不能准确地描述这些动态.
- 空间分辨率技术对于全面了解表面反应至关重要.
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