Imaging Catalytic Hotspots on Single Plasmonic Nanostructures via Correlated Super-Resolution and Electron Microscopy,ACS Nano

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Imaging Catalytic Hotspots on Single Plasmonic Nanostructures via Correlated Super-Resolution and Electron Microscopy
ACS Nano ( IF 15.8 ) Pub Date : 2018-06-04 00:00:00 , DOI: 10.1021/acsnano.8b01338
Ningmu Zou ₁ , Guanqun Chen ₁ , Xianwen Mao ₁ , Hao Shen ₁ , Eric Choudhary ₁ , Xiaochun Zhou ₁ , Peng Chen ₁

Affiliation

Surface-plasmon (SP) enhanced catalysis on plasmonic nanostructures brings opportunities to increase catalytic efficiency and alter catalytic selectivity. Understanding the underlying mechanism requires quantitative measurements of catalytic enhancement on these nanostructures, whose intrinsic structural heterogeneity presents experimental challenges. Using correlated super-resolution fluorescence microscopy and electron microscopy, here we report a quantitative visualization of SP-enhanced catalytic activity at the nanoscale within single plasmonic nanostructures. We focus on two Au- and Ag-based linked nanostructures that present plasmonic hotspots at nanoscale gaps. Spatially localized higher reaction rates at these gaps vs nongap regions report the SP-induced catalytic enhancements, which show direct correlations with the nanostructure geometries and local electric field enhancements. Furthermore, the catalytic enhancement scales quadratically with the local actual light intensity, attributable to hot electron involvement in the catalytic enhancement mechanism. These discoveries highlight the effectiveness of correlated super-resolution and electron microscopy in interrogating nanoscale catalytic properties.

中文翻译：

通过相关的超分辨率和电子显微镜成像单个等离子体纳米结构上的催化热点。

表面等离激元（SP）在等离激元纳米结构上的增强催化作用提供了增加催化效率和改变催化选择性的机会。要了解潜在的机理，就需要对这些纳米结构上的催化增强进行定量测量，其内在的结构异质性给实验带来了挑战。使用相关的超分辨率荧光显微镜和电子显微镜，这里我们报告了单等离子体纳米结构内纳米级SP增强的催化活性的定量可视化。我们专注于两个基于Au和Ag的链接纳米结构，这些纳米结构在纳米级间隙呈现等离激元热点。与非空位区域相比，这些空位在空间上的局部反应速率更高，表明SP诱导了催化作用的增强，它们显示出与纳米结构的几何形状和局部电场增强的直接相关性。此外，归因于热电子参与催化增强机理，催化增强与局部实际光强度呈二次方关系。这些发现突出了相关的超分辨率和电子显微镜在询问纳米级催化性能方面的有效性。

更新日期：2018-06-04

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