Mechanisms of Nucleation and Stationary States of Electrochemically Generated Nanobubbles

成核 化学物理 化学 耗散系统 电流(流体) 过饱和度 电极 气泡 分子动力学 纳米技术 机械 热力学 材料科学 计算化学 物理化学 物理 有机化学
作者
Yamila A. Perez Sirkin,Esteban D. Gadea,Damián A. Scherlis,Valeria Molinero
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:141 (27): 10801-10811 被引量:112
标识
DOI:10.1021/jacs.9b04479
摘要

Gas evolving reactions are ubiquitous in the operation of electrochemical devices. Recent studies of individual gas bubbles on nanoelectrodes have resulted in unprecedented control and insights on their formation. The experiments, however, lack the spatial resolution to elucidate the molecular pathway of nucleation of nanobubbles and their stationary size and shape. Here we use molecular simulations with an algorithm that mimics the electrochemical formation of gas, to investigate the mechanisms of nucleation of gas bubbles on nanoelectrodes, and characterize their stationary states. The simulations reproduce the experimental currents in the induction and stationary stages, and indicate that surface nanobubbles nucleate through a classical mechanism. We identify three distinct regimes for bubble nucleation, depending on the binding free energy per area of bubble to the electrode, Δγbind. If Δγbind is negative, the nucleation is heterogeneous and the nanobubble remains bound to the electrode, resulting in a low-current stationary state. For very negative Δγ, the bubble fully wets the electrode, forming a one-layer-thick micropancake that nucleates without supersaturation. On the other hand, when Δγbind > 0 the nanobubble nucleates homogeneously close to the electrode, but never attaches to it. We conclude that all surface nanobubbles must nucleate heterogeneously. The simulations reveal that the size and contact angle of stationary nanobubbles increase with the reaction driving force, although their residual current is invariant. The myriad of driven nonequilibrium stationary states with the same rate of production of gas, but distinct bubble properties, suggests that these dissipative systems have attractors that control the stationary current.
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