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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Penetration of Platinum Complex Anions into Porous Silicon: Anomalous Behavior Caused by Surface-Induced Phase Transition
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Penetration of Platinum Complex Anions into Porous Silicon: Anomalous Behavior Caused by Surface-Induced Phase Transition

机译：铂络合物阴离子渗透到多孔硅中：表面诱导的相变引起的异常行为

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摘要

We investigate the dynamics of the penetration of platinum complex anions into nanopores during platinum deposition within a nanoporous silicon electrode. The pore-wall surface is hydrophobic and the anions are large enough to behave like hydrophobic solutes. Some of the observations are anomalous in the sense that they cannot be understood in terms of the phenomenological theory for diffusion based on Fick's law. For example, the penetration is faster when the pore diameter is smaller and the anion size is larger. The penetration rate remains unexpectedly fast even when the pores become deeper. The penetration can be made faster using large coexisting cations with sufficiently high hydrophobicity. We show that these results can be interpreted only by statistical mechanics of confined molecular liquids. When the manipulated variables (pore diameter, anion concentration, sizes of platinum complex anions and coexisting cations, etc.) are chosen so that the surface-induced phase transition (SIFT) can take place, the penetration is drastically accelerated. Under the condition with the SIFT occurrence, a strongly attractive, long-ranged effective surface anion interaction comes into play, leading to the anomalous behavior. The experimental result is in qualitatively good accord with the theoretical argument. The outcome is of vital importance in controlling the mass transfer within nanoporous media and designing next-generation electrochemical devices.
机译：我们调查在纳米孔硅电极内铂沉积过程中铂络合物阴离子渗透到纳米孔中的动力学。孔壁表面是疏水性的，阴离子足够大，表现得像疏水性溶质。从基于菲克定律的扩散现象学理论无法理解的意义上讲，有些观察是异常的。例如，当孔径较小且阴离子尺寸较大时，渗透速度更快。即使毛孔变深，渗透率仍然保持出乎意料的快。使用具有足够高疏水性的大的共存阳离子可以使渗透更快。我们表明，这些结果只能由受限分子液体的统计力学来解释。选择操纵变量（孔径，阴离子浓度，铂络合物阴离子的大小和共存阳离子等）以使发生表面诱导的相变（SIFT）时，渗透速度会大大加快。在发生SIFT的条件下，强烈吸引人的，长期有效的表面阴离子相互作用开始起作用，从而导致异常行为。实验结果在质量上与理论观点相吻合。结果对于控制纳米多孔介质内的传质和设计下一代电化学装置至关重要。

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