James Martin David, Decarolis Donato, Odarchenko Yaroslav I, Herbert Jennifer J, Arnold Thomas, Rawle Jonathan, Nicklin Chris, Boyen Hans-Gerd, Beale Andrew M
Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ, UK.
Diamond Light Source, Harwell Science and Innovation Campus, Chilton, Didcot OX11 0DE, UK.
Chem Commun (Camb). 2017 May 4;53(37):5159-5162. doi: 10.1039/c7cc01887h.
Periodically arranged, monodisperse gold nanoparticles supported on flat silicon substrates were studied for the hydrogenation of 1,3-butadiene under operando conditions using Grazing Incidence Small- and Wide-Angle X-ray Scattering (GISAXS/GIWAXS). It was found that the composition and shape of the nanoparticles depends very much on the chemical environment; the particles are shown to be dynamic, undergoing reversible size and shape change particularly during catalytic reaction, highlighting a dynamism often not observed in traditional studies. Specifically, the size of the Au nanoparticles increases during butadiene hydrogenation and this is attributed to the partial removal of a AuO at the metal-oxide interface and consequential shape change of the nanoparticle from a more hemispherical particle to a particle with a larger height to width ratio.
使用掠入射小角和广角X射线散射（GISAXS/GIWAXS）技术，在操作条件下研究了负载在平坦硅衬底上的周期性排列的单分散金纳米颗粒对1,3 - 丁二烯的氢化作用。研究发现，纳米颗粒的组成和形状在很大程度上取决于化学环境；结果表明这些颗粒具有动态性，尤其是在催化反应过程中会经历可逆的尺寸和形状变化，这突出了传统研究中常常未观察到的动态特性。具体而言，在丁二烯氢化过程中，金纳米颗粒的尺寸会增大，这归因于金属 - 氧化物界面处的AuO部分去除，以及纳米颗粒随之从更接近半球形的颗粒转变为高宽比更大的颗粒。
