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用于平行单颗粒催化的面心胶体纳米晶体的纳流控捕获。

Nanofluidic Trapping of Faceted Colloidal Nanocrystals for Parallel Single-Particle Catalysis.

机构信息

Department of Biology and Biological Engineering, Chalmers University of Technology; SE-412 96 Gothenburg, Sweden.

Department of Chemistry and Chemical Engineering, Chalmers University of Technology; SE-412 96 Gothenburg, Sweden.

出版信息

ACS Nano. 2022 Sep 27;16(9):15206-15214. doi: 10.1021/acsnano.2c06505. Epub 2022 Sep 2.

Abstract

Catalyst activity can depend distinctly on nanoparticle size and shape. Therefore, understanding the structure sensitivity of catalytic reactions is of fundamental and technical importance. Experiments with single-particle resolution, where ensemble-averaging is eliminated, are required to study it. Here, we implement the selective trapping of individual spherical, cubic, and octahedral colloidal Au nanocrystals in 100 parallel nanofluidic channels to determine their activity for fluorescein reduction by sodium borohydride using fluorescence microscopy. As the main result, we identify distinct structure sensitivity of the rate-limiting borohydride oxidation step originating from different edge site abundance on the three particle types, as confirmed by first-principles calculations. This advertises nanofluidic reactors for the study of structure-function correlations in catalysis and identifies nanoparticle shape as a key factor in borohydride-mediated catalytic reactions.

摘要

催化剂的活性可以明显依赖于纳米粒子的尺寸和形状。因此,了解催化反应的结构敏感性具有基础和技术上的重要意义。需要进行具有单粒子分辨率的实验,以消除集合平均。在这里,我们在 100 条平行的纳米流道中实现了对单个球形、立方和八面体胶体金纳米晶体的选择性捕获,以使用荧光显微镜确定它们对硼氢化钠还原荧光素的活性。作为主要结果,我们确定了三种粒子类型上不同边缘位置丰度导致的限速硼氢化钠氧化步骤的明显结构敏感性,这一点通过第一性原理计算得到了证实。这为在纳米流道反应器中研究催化中的结构-功能相关性提供了信息,并确定了纳米粒子形状是硼氢化介导的催化反应中的一个关键因素。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8ef9/9527799/6bd475662595/nn2c06505_0001.jpg

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