We report a unique in situ instrument development effort dedicated to studying gas/solid interactions relevant to heterogeneous catalysis and early stages of oxidation of materials via atom probe tomography and microscopy (APM). An in situ reactor cell, similar in concept to other reports, has been developed to expose nanoscale volumes of material to reactive gas environments, in which temperature, pressure, and gas chemistry are well controlled. We demonstrate that the combination of this reactor cell with APM techniques can aid in building a better mechanistic understanding of resultant composition and surface and subsurface structure changes accompanying gas/surface reactions in metal and metal alloy systems through a series of case studies: O₂/Rh, O₂/Co, and O₂/Zircaloy-4. In addition, the basis of a novel operando mode of analysis within an atom probe instrument is also reported. The work presented here supports the implementation of APM techniques dedicated to atomic to near-atomically resolved gas/surface interaction studies of materials broadly relevant to heterogeneous catalysis and oxidation.

我们报告了一项独特的原位仪器开发工作，该工作致力于通过原子探针层析成像和显微镜（APM）研究与多相催化和材料氧化早期有关的气/固相互作用。已经开发了概念上与其他报告类似的原位反应器电池，以将纳米级体积的材料暴露于反应性气体环境中，在该环境中温度，压力和气体化学反应得到了很好的控制。我们证明了该反应堆电池与APM技术的结合可以通过一系列案例研究，帮助建立对伴随金属和金属合金系统中的气体/表面反应而产生的成分以及表面和地下结构变化的更好的机械理解：O ₂ / Rh，O ₂ / Co和O ₂/ Zircaloy-4。另外，还报道了在原子探针仪器内新颖的操作模式分析的基础。本文介绍的工作支持APM技术的实施，该技术专门用于与异质催化和氧化广泛相关的材料的原子至近原子分辨的气体/表面相互作用研究。