论文标题

用原子探针层析成像直接成像液 - 纳米粒子界面

Direct imaging of liquid-nanoparticle interface with atom probe tomography

论文作者

Qiu, Shi., Zheng, Changxi, Zhou, Qi, Dong, Dashen, Shi, Qianqian, Garg, Vivek, Zhang, Shuo, Cheng, Wenlong, Marceau, Ross K. W., Sha, Gang, Fu, Jing

论文摘要

了解液 - 纳米颗粒(NP)界面的结构和化学组成对于广泛的物理,化学和生物学过程至关重要。在这项研究中,首次报道了通过原子探针断层扫描(APT)对液体NP界面进行直接成像,这揭示了该关键域中关键原子和分子的分布和相互作用。 APT试样是通过对金属尖端上含有纳米颗粒的溶液的控制的石墨烯封装来制备的,末端半径在50 nm的范围内,以允许场电离和蒸发。以悬浮液为例,以Au纳米颗粒(AUNP)为例,对APT的质谱和三维(3D)化学图的分析提供了具有近原子分辨率的水金界面的详细图像。在水金界面上,已经观察到了富含水(H2O)分子的电气双层(EDL)的形成,这是由硫酸三氧化三肽层和AUNP之间的结合产生的。在散装水区域,已显示重建的H2O的密度是一致的,反映了石墨烯封装后H2O分子的高度密度。这项研究是使用APT与apt的结果进行直接成像的首次演示,从而提供了液体-NP界面的原子3D解剖。

Understanding the structure and chemical composition at the liquid-nanoparticle (NP) interface is crucial for a wide range of physical, chemical and biological processes. In this study, direct imaging of the liquid-NP interface by atom probe tomography (APT) is reported for the first time, which reveals the distributions and the interactions of key atoms and molecules in this critical domain. The APT specimen is prepared by controlled graphene encapsulation of the solution containing nanoparticles on a metal tip, with an end radius in the range of 50 nm to allow field ionization and evaporation. Using Au nanoparticles (AuNPs) in suspension as an example, analysis of the mass spectrum and three-dimensional (3D) chemical maps from APT provides a detailed image of the water-gold interface with near-atomic resolution. At the water-gold interface, the formation of an electrical double layer (EDL) rich in water (H2O) molecules has been observed, which results from the charge from the binding between the trisodium-citrate layer and the AuNP. In the bulk water region, the density of reconstructed H2O has been shown to be consistent, reflecting a highly packed density of H2O molecules after graphene encapsulation. This study is the first demonstration of direct imaging of liquid-NP interface using APT with results providing an atom-by-atom 3D dissection of the liquid-NP interface.

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