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Impact and oxidation of single silver nanoparticles at electrode surfaces: one shot versus multiple events

机译：单个银纳米颗粒在电极表面的撞击和氧化：一次撞击与多次撞击

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Single nanoparticle (NP) electrochemical impacts is a rapidly expanding field of fundamental electrochemistry, with applications from electrocatalysis to electroanalysis. These studies, which involve monitoring the electrochemical (usually current–time, I–t) response when a NP from solution impacts with a collector electrode, have the scope to provide considerable information on the properties of individual NPs. Taking the widely studied oxidative dissolution of individual silver nanoparticles (Ag NPs) as an important example, we present measurements with unprecedented noise (< 5 pA) and time resolution (time constant 100 μs) that are highly revealing of Ag NP dissolution dynamics. Whereas Ag NPs of diameter, d = 10 nm are mostly dissolved in a single event (on the timescale of the measurements), a wide variety of complex processes operate for NPs of larger diameter (d ≥ 20 nm). Detailed quantitative analysis of the I–t features, consumed charge, event duration and impact frequency leads to a major conclusion: Ag NPs undergo sequential partial stripping (oxidative dissolution) events, where a fraction of a NP is electrochemically oxidized, followed by the NP drifting away and back to the tunnelling region before the next partial stripping event. As a consequence, analysis of the charge consumed by single events (so-called “impact coulometry”) cannot be used as a general method to determine the size of colloidal NPs. However, a proper analysis of the I–t responses provides highly valuable information on the transient physicochemical interactions between NPs and polarized surfaces.
机译：单个纳米颗粒（NP）的电化学影响是基础电化学领域的快速扩展，其应用范围从电催化到电分析。这些研究涉及监测溶液中的NP撞击集电极时的电化学响应（通常为电流-时间，IT响应），具有提供有关各个NP性质的大量信息的范围。以广泛研究的单个银纳米颗粒（Ag NPs）的氧化溶解为重要示例，我们提出了具有前所未有的噪声（<5 pA）和时间分辨率（时间常数100μs）的测量方法，这些测量值高度揭示了Ag NP溶解动力学。直径为d = 10 nm的Ag NPs大多在一次事件中溶解（在测量的时间尺度上），而直径较大（d≥20 nm）的NPs则有各种各样的复杂过程。对It特性，消耗的电荷，事件持续时间和撞击频率的详细定量分析得出一个主要结论：Ag NP经历了顺序的部分汽提（氧化溶解）事件，其中一部分NP被电化学氧化，随后是NP在下一次部分剥离事件之前漂移并返回到隧道区域。结果，对单个事件消耗的电荷的分析（所谓的“碰撞库仑法”）不能用作确定胶体NP大小的通用方法。但是，对I–t反应的正确分析提供了有关NP与极化表面之间瞬态物理化学相互作用的极有价值的信息。

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