Direct Observations of Electrochemical Reactions within Au-YSZ Thin Films via Absorption Shifts in the Au Nanoparticle Surface Plasmon Resonance

Direct Observations of Electrochemical Reactions within Au-YSZ Thin Films via Absorption Shifts in the Au Nanoparticle Surface Plasmon Resonance
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通过 Au 纳米颗粒表面等离子共振的吸收位移直接观察 Au-YSZ 薄膜内的电化学反应

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发表时间:
2008
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通讯作者:
M. Carpenter
M. Carpenter
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作者:
P. Rogers;G. Sirinakis;M. Carpenter

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在 500°C、不同浓度的 N2 中的 H2 和 O2 气体暴露下,对嵌入 YSZ 基质中的 Au 纳米粒子的表面等离子共振 (SPR) 谱带进行监测。由于SPR带的峰值位置密切依赖于每个金纳米颗粒驱动振荡自由电子的数量,因此我们能够通过监测Au−YSZ纳米复合薄膜的光学性质,特别是SPR带的峰值位置来监测从Au纳米颗粒到扩散氧离子的电化学电荷转移。观察到平衡比 pH21/4/pO21/8 的变化(有助于氧离子扩散进出 YSZ 基质)和 SPR 带峰值位置的平方变化之间存在直接关系。自由电子理论指出,SPR 带峰值位置的平方变化与每个金纳米粒子可用的传导电子的变化成正比;因此,我们的观察结果与电荷转移与氧化还原气体的预期趋势一致......
The surface plasmon resonance (SPR) band of Au nanoparticles embedded in an YSZ matrix was monitored at 500 °C under varying gas exposure concentrations of H2 and O2 in N2. Because the peak position of the SPR band relies closely on the number of driven oscillating free electrons per gold nanoparticle, we were able to monitor electrochemical charge transfer from Au nanoparticles to diffusing oxygen ions by monitoring the optical properties of the Au−YSZ nanocomposite thin film, specifically the peak position of the SPR band. A direct relation was observed for the change in the equilibrium ratio, pH21/4/pO21/8, contributing to oxygen ion diffusion into and out of the YSZ matrix, and the change in the square of the SPR band peak position. Free electron theory states that this change in the square of the SPR band peak position is directly proportional to the change in conduction electrons available per Au nanoparticle; thus, our observations agree with the expected trend for charge transfer vs the redox gas ...