外延薄膜作为理解组分复杂的电催化剂模型平台
Epitaxial Films as Model Platform for Understanding Compositionally Complex Electrocatalysts
AI总结：
本文提出外延薄膜作为研究组分复杂电催化剂的模型平台，通过纳米尺度结构-活性映射实现了电催化剂的合理设计。
摘要：
组分复杂的固溶体提供了一种独特的途径来工程高性能电催化剂，其中多元素表面组分可以无缝调节以优化活性、选择性和稳定性。然而，这些电催化剂的机理理解仍然受到缺乏具有晶格定义表面且能与相关、多尺度表征相容的模型系统限制。本文提出外延薄膜作为研究组分复杂电催化剂的模型平台。通过磁控溅射，我们利用(111)Pt缓冲层在(0001) Sapphire基底上实现了(111)外延Ir-Pd-Pt-Rh-Ru薄膜，通过X射线衍射和透射电子显微镜确认。该生长方法适用于广泛组成范围，产生平滑表面（均方根粗糙度<1nm）并在纳米尺度薄膜中产生微米级晶粒。利用这些薄膜，我们通过微-indent和进行相关原子力显微镜、电子背散射衍射和扫描电化学细胞显微镜实现了纳米尺度的结构-活性映射。我们的工作建立了一个用于基础尺度桥接表征的模型平台，并为组分复杂电催化剂的合理设计铺平了道路。
英文摘要：
Compositionally complex solid solutions provide a unique route for engineering high-performance electrocatalysts, where the polyelemental surface composition can be seamlessly tuned to optimize activity, selectivity, and stability. However, the mechanistic understanding of these electrocatalysts remains limited by the lack of a model system with a crystallographically-defined surface that is compatible with correlative, multi-scale characterization. Here, we present epitaxial films as a model platform for studying compositionally complex electrocatalysts. Using magnetron sputtering, we realize (111) epitaxial Ir-Pd-Pt-Rh-Ru films on (0001) sapphire substrate via a (111) Pt buffer layer, confirmed by X-ray diffraction and transmission electron microscopy. The growth approach is applicable across a broad composition range and produces smooth surfaces (root mean square roughness < 1 nm) with micrometer-sized grains in the nanoscale films. With these films, we demonstrate direct structure-activity mapping at the nanoscale through precise co-localization using micro-indents and performing correlative atomic force microscopy, electron backscatter diffraction, and scanning electrochemical cell microscopy. Our work establishes a model platform for fundamental scalebridging characterization and paves the way for rational design of compositionally complex electrocatalysts.
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