Institute of Experimental Physics, Graz University of Technology, Graz, Austria.
Institute for Electron Microscopy and Nanoanalysis, Graz University of Technology, Graz, Austria.
Faraday Discuss. 2023 Jan 31;242(0):160-173. doi: 10.1039/d2fd00089j.
Nanoparticles with diameters in the range of a few nanometers, consisting of gold and vanadium oxide, are synthesized by sequential doping of cold helium droplets in a molecular beam apparatus and deposited on solid carbon substrates. After surface deposition, the samples are removed and various measurement techniques are applied to characterize the created particles: scanning transmission electron microscopy (STEM) at atomic resolution, temperature dependent STEM and TEM up to 650 °C, energy-dispersive X-ray spectroscopy (EDXS) and electron energy loss spectroscopy (EELS). In previous experiments we have shown that pure VO nanoparticles can be generated by sublimation from the bulk and deposited without affecting their original stoichiometry. Interestingly, our follow-up attempts to create Au@VO core@shell particles do not yield the expected encapsulated structure. Instead, Janus particles of Au and VO with diameters between 10 and 20 nm are identified after deposition. At the interface of the Au and the VO parts we observe an epitaxial-like growth of the vanadium oxide next to the Au structure. To test the temperature stability of these Janus-type particles, the samples are heated during the STEM measurements from room temperature up to 650 °C, where a reduction from VO to VO is followed by a restructuring of the gold atoms to form a Wulff-shaped cluster layer. The temperature dependent dynamic interplay between gold and vanadium oxide in structures of only a few nanometer size is the central topic of this contribution to the Faraday Discussion.
粒径在几纳米范围内的纳米粒子,由金和氧化钒组成,通过在分子束装置中顺序掺杂冷氦液滴合成,并沉积在固体碳基底上。表面沉积后,将样品取出,并应用各种测量技术对所创建的粒子进行表征:原子分辨率的扫描透射电子显微镜(STEM)、温度依赖的 STEM 和 TEM 最高可达 650°C、能量色散 X 射线光谱(EDXS)和电子能量损失光谱(EELS)。在之前的实验中,我们已经表明,纯 VO 纳米粒子可以通过从体相升华并沉积而不影响其原始化学计量比来生成。有趣的是,我们后续尝试创建 Au@VO 核壳粒子的尝试并未产生预期的封装结构。相反,沉积后会识别出直径在 10 至 20nm 之间的 Au 和 VO 的 Janus 粒子。在 Au 和 VO 部分的界面处,我们观察到氧化钒在 Au 结构旁边的外延样生长。为了测试这些 Janus 型粒子的温度稳定性,在 STEM 测量过程中,样品从室温加热到 650°C,其中 VO 到 VO 的还原伴随着金原子的重构,形成 Wulff 形状的团簇层。在只有几纳米大小的结构中,金和氧化钒之间的温度依赖的动态相互作用是本论文的核心主题。