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arXiv physics/0210105physics.chem-ph
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化学反应控制下的非均匀形核-电流瞬态

Heterogeneous nucleation - current transients under chemical reaction control

P. C. T. Dajello, I. Mozolevski, Z. G. S. Kipervaser

摘要:

通过一个随机模型描述了催化剂表面上的非均质成核。为了产生这种非平衡过程,我们假设静电势的开启触发复杂的动力学,其包括自由布朗运动、反应动力学和在离子最终粘附在表面(电极)上之前的受激迁移。在,当电位被打开时,空间对称性被破坏,并发展出两阶段过程。首先,离子在其电化学特性上发生变化(在空间的某些区域),然后在某些特定点发生反应,在表面上粘在一起。离子的连续添加产生与电化学沉积过程中测量的电流瞬态信号相关的材料沉积。与文献中发现的当前模型不同,该过程避免了计算扩散区所覆盖的面积,允许形式主义技巧同样很好地描述带电表面上的通道对离子的吸收。该理论适用于电沉积镍在n-硅和解释失败的标准三维成核模型重现的情况下,界面关系控制的动态。结果表明,在电极上的化学反应占主导地位的过程不能被归类为拥有一个专门的瞬时或渐进的字符,而是,他们混合在一起,这两种限制形式的核激活,以定义在其开始的电流瞬变。

英文摘要:

Heterogeneous nucleation on catalytic surfaces plunged into a fluid is described through a stochastic model. To generate this non-equilibrium process we assume that the turn on of a electrostatic potential triggers a complex dynamics that includes a free Brownian motion, a reaction kinetic and a stimulated migration before the final adhesion of ions on the surface (electrode). At, when the potential is switched on, the spatial symmetry is broken and a two-stage process is developed. First the ion undergoes a change in its electrochemical character (at some region of the space) and then reacts at some specific points to stick together on the surface. The continuous addition of ions develops a material deposit connected to the current transient signals measured in electrochemical deposition processes. Unlike current models found in the literature, this procedure avoids the computation of the area covered by the diffusion zones, allowing a formalism skill to describe equally well the absorption of ions by channels on electrified surfaces. The theory is applied to the electrodeposition of nickel on n-silicon and explains the failure of standard three-dimensional nucleation models to reproduce situations where interfacial relations control the dynamics. It is shown that, processes dominated by chemical reactions on the electrode can not be classified as possessing an exclusively instantaneous or progressive character, rather, they mix together these two limiting forms of nuclei activation to defines the current transients in its beginning.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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