超高分辨率催化成像技术可视化单一纳米催化剂的双金属作用,ACS Central Science

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超高分辨率催化成像技术可视化单一纳米催化剂的双金属作用
ACS Central Science ( IF 12.7 ) Pub Date : 2017-11-01 00:00:00 , DOI: 10.1021/acscentsci.7b00377
Guanqun Chen ₁ , Ningmu Zou ₁ , Bo Chen ₁ , Justin B. Sambur ₁ , Eric Choudhary ₁ , Peng Chen ₁

Affiliation

与它们的单金属对应物相比，双金属纳米颗粒通常显示出与双金属界面相关的增强的催化活性。对双金属界面催化活性的直接定量对于理解增强机理很重要，但在实验上具有挑战性。在这里使用与电子显微镜相关的单分子超分辨率催化成像，我们报告了单个双金属纳米颗粒内增强的双金属活性的第一个定量可视化。我们关注于异核双金属PdAu纳米粒子，它们在催化光致荧光歧化反应中表现出明确的Pd-Au双金属界面。我们的方法还可以直接比较同一纳米粒子中的双金属和单金属区域。理论计算进一步洞察了吸附在双金属位点上的反应物（刃天青）的N-O键活化的电子性质。双金属增强与单金属活性之间的亚颗粒活性相关性表明，构建双金属位点的有利位置是那些具有较高活性的单金属位点，从而导致了制备有效的双金属纳米催化剂的策略。结果突出了超分辨率催化成像在获得有助于改善纳米催化剂的见解方面的力量。双金属增强与单金属活性之间的亚颗粒活性相关性表明，构建双金属位点的有利位置是那些具有较高活性的单金属位点，从而导致了制备有效的双金属纳米催化剂的策略。结果突出了超分辨率催化成像在获得有助于改善纳米催化剂的见解方面的力量。双金属增强与单金属活性之间的亚颗粒活性相关性表明，构建双金属位点的有利位置是那些具有较高活性的单金属位点，从而导致了制备有效的双金属纳米催化剂的策略。结果突出了超分辨率催化成像在获得有助于改善纳米催化剂的见解方面的力量。

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Bimetallic Effect of Single Nanocatalysts Visualized by Super-Resolution Catalysis Imaging

Compared with their monometallic counterparts, bimetallic nanoparticles often show enhanced catalytic activity associated with the bimetallic interface. Direct quantitation of catalytic activity at the bimetallic interface is important for understanding the enhancement mechanism, but challenging experimentally. Here using single-molecule super-resolution catalysis imaging in correlation with electron microscopy, we report the first quantitative visualization of enhanced bimetallic activity within single bimetallic nanoparticles. We focus on heteronuclear bimetallic PdAu nanoparticles that present a well-defined Pd–Au bimetallic interface in catalyzing a photodriven fluorogenic disproportionation reaction. Our approach also enables a direct comparison between the bimetallic and monometallic regions within the same nanoparticle. Theoretical calculations further provide insights into the electronic nature of N–O bond activation of the reactant (resazurin) adsorbed on bimetallic sites. Subparticle activity correlation between bimetallic enhancement and monometallic activity suggests that the favorable locations to construct bimetallic sites are those monometallic sites with higher activity, leading to a strategy for making effective bimetallic nanocatalysts. The results highlight the power of super-resolution catalysis imaging in gaining insights that could help improve nanocatalysts.

更新日期：2017-11-22

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