Correlating Surface Structures and Electrochemical Activity Using Shape-Controlled Single-Pt Nanoparticles
Correlating Surface Structures and Electrochemical Activity Using Shape-Controlled Single-Pt Nanoparticles
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DOI：
10.1021/acsnano.1c06281
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发表时间：
2021-11-23
期刊：
影响因子：
17.1
通讯作者：
Crooks, Richard M.
中科院分区：
文献类型：
--
作者：
Huang, Ke;Shin, Kihyun;Crooks, Richard M.
我们报告了一种合成和研究形状控制的，单铂纳米粒子（NPs）支持在碳纳米电极的方法。关键的进步是，合成方法可以生产具有广泛晶体结构和尺寸的单一电化学活性NP。同样重要的是，NP可以被完全表征，并且因此NP的电化学性质可以与单个形状的尺寸和结构直接相关。这使得直接将实验结果与第一原理理论联系起来成为可能。由于每次仅分析一个良好表征的NP，因此避免了将理论分析应用于具有不同尺寸和结构的NP的集合的困难。在这篇文章中，我们报告了两个特定的Pt NP形状的大小为200 nm的顺序：凹六八面体（HOH）和凹八面体（TPH）。前者有{1561}面，后者有{1011}面。这些单纳米颗粒的甲酸氧化（FAO）反应的电化学性能进行比较，一个单一的，球形多晶Pt NP相同的大小。最后，密度泛函理论，进行电化学研究之前，被用来解释FAO实验的实验结果。
We report a method for synthesizing and studying shape-controlled, single Pt nanoparticles (NPs) supported on carbon nanoelectrodes. The key advance is that the synthetic method makes it possible to produce single, electrochemically active NPs with a vast range of crystal structures and sizes. Equally important, the NPs can be fully characterized, and, therefore, the electrochemical properties of the NPs can be directly correlated to the size and structure of a single shape. This makes it possible to directly correlate experimental results to first-principles theory. Because just one well-characterized NP is analyzed at a time, the difficulty of applying a theoretical analysis to an ensemble of NPs having different sizes and structures is avoided. In this article, we report on two specific Pt NP shapes having sizes on the order of 200 nm: concave hexoctahedral (HOH) and concave trapezohedral (TPH). The former has {1561} facets and the latter {1011} facets. The electrochemical properties of these single NPs for the formic acid oxidation (FAO) reaction are compared to those of a single, spherical polycrystalline Pt NP of the same size. Finally, density functional theory, performed prior to the electrochemical studies, were used to interpret the experimental results of the FAO experiments.