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首页> 外文期刊>Catalysis science & technology >Determining intrinsic stark tuning rates of adsorbed CO on copper surfaces
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Determining intrinsic stark tuning rates of adsorbed CO on copper surfaces

机译：确定内在的调优率吸附在铜表面

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The abrupt change in potential between the electrode and the electrolyte, and the resulting interfacial electric field, is the driving force in electrochemical reactions. For surface mediated electrocatalytic reactions, the interfacial electric field is believed to have a key impact on the stability and reactivity of adsorbed intermediates. However, the exact mechanisms remain a topic of discussion. In this context, reliable measurements of the interfacial electric field are a prerequisite in understanding how it influences the rate and product distribution in electrochemical reactions. The vibrational Stark effect of adsorbates, such as CO, offers an accessible means to assess the interfacial electric field strength by determining the shift of vibrational peaks of the adsorbates with potential, i.e., the Stark tuning rate. However, the vibrational Stark effect could be convoluted with the dynamical dipole coupling effect of the adsorbates on weak binding surfaces such as Cu, thus complicating the determination of the intrinsic Stark tuning rate. In this work, we report a general and effective strategy of determining the intrinsic Stark tuning rate by removing the impact of the dynamical coupling of adsorbed CO on the Cu surface with surface enhanced infrared absorption spectroscopy. A similar intrinsic Stark tuning rate of similar to 33 cm V-1 was obtained on oxide-derived Cu in different electrolyte pH of 7.2, 10.9 and 12.9, indicating the pH independence of the interfacial electric field. Investigations on different Cu electrodes show that the intrinsic Stark tuning rates on (electro)chemically deposited films are close to 33 cm V-1, while particulate Cu catalysts show a similar value of similar to 68 cm V-1. These observations indicate that aggregate morphology, rather than the size and shape of individual catalyst particles, has a more prominent impact on the interfacial electric field.
机译：之间的潜在的突然改变电极和电解质,以及由此产生的界面电场的驱动力在电化学反应。介导electrocatalytic反应,界面电场被认为有一个主要对的稳定性和反应性的影响吸附中间体。机制仍然是一个讨论的话题。背景下,可靠的测量界面电场是一个先决条件它如何影响率和理解产品分布在电化学反应。被吸附物,如有限公司提供了一个访问意味着评估界面电场力量通过确定振动的转变山峰被吸附物的潜力,即鲜明的调优率。与动力效应可能是复杂的被吸附物的偶极耦合效应弱绑定表面,如铜,因此复杂化内在的决心的调优率。确定固有的有效策略鲜明的调优率通过消除的影响动力耦合吸附CO的铜表面与表面增强红外吸收光谱学。率与它们类似于33厘米了oxide-derived铜在不同电解液的pH值7.2、10.9和12.9,表明pH值独立的界面电场。调查显示在不同的铜电极内在的调整利率(电)化学沉积电影接近它们完全33厘米,而颗粒铜催化剂显示相似的类似于68厘米与它们的价值。观察结果表明,聚合形态,而不是个人的大小和形状催化剂粒子,有更重要的影响在界面电场。

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