A multimodal chemical imaging approach has been developed and applied to detail the dynamic, atomic-scale changes associated with oxidation of a zirconium alloy (Zircaloy-4). Scanning transmission electron microscopy, a gas-phase reactor chamber attached to an atom probe tomography instrument, and synchrotron-based X-ray absorption near-edge spectroscopy were employed to reveal morphology, composition, crystal, and electronic structure changes that occur during initial stages of oxidation at 300 °C. Oxidation was carried out in 10 mbar O₂ gas for short exposure times of 1 and 5 min. A multilayered oxide film with a cubic ZrO adjacent to the oxide/metal interface, a nanoscopic transition region with a graded composition of ZrO_2−x (where 0 < x < 1), and tetragonal ZrO₂ in the outermost oxide were formed. Partitioning of the major alloying element (tin) to the oxide/metal interface and heterogeneously within the oxide accompanied the development of the layered oxide. Our work provides a rapid, high-throughput approach for detailed characterisation of initial stages of zirconium alloy oxidation at an accelerated time scale, with implications for several other alloy systems.

已开发出一种多峰化学成像方法，并将其应用于详细描述与锆合金（Zircaloy-4）氧化有关的动态原子级变化。扫描透射电子显微镜，连接到原子探针断层扫描仪的气相反应器室以及基于同步加速器的X射线吸收近边缘光谱仪可揭示初始阶段发生的形貌，组成，晶体和电子结构变化300°C下的氧化反应。在10 mbar O ₂气体中进行氧化，暴露时间为1分钟和5分钟。具有与氧化物/金属界面相邻的立方ZrO的多层氧化膜，具有ZrO _{2- x}（其中0 <  x ＜1），并且在最外层氧化物中形成四方ZrO ₂。主要合金元素（锡）在氧化物/金属界面上的分配以及在氧化物内的不均匀分配伴随着层状氧化物的发展。我们的工作提供了一种快速，高通量的方法，用于在加速的时间尺度上详细表征锆合金氧化的初始阶段，这对其他几种合金系统也具有重要意义。