材料科学
氧还原反应
催化作用
合金
纳米结构
氧还原
化学工程
纳米技术
表面改性
曲面(拓扑)
Crystal(编程语言)
冶金
物理化学
有机化学
电化学
化学
几何学
数学
电极
计算机科学
工程类
程序设计语言
作者
Yoshihiro Chida,Sae Dieb,H. Masui,Arata Umehara,Keitaro Sodeyama,Toshimasa Wadayama
标识
DOI:10.1021/acsami.4c22052
摘要
We investigated oxygen reduction reaction (ORR) properties of Pt-containing compositionally complex alloy (Pt-CCA) single-crystal model catalyst surfaces to optimize dry-process synthesis conditions, that is, CCA compositions of less-noble alloying elements and their synthesis (annealing) temperatures. Using a machine-learning approach, we effectively navigated the large space of possible synthesis conditions to minimize the experimental workload. The ORR activity and durability of the Pt/CCA/Pt(111) model catalyst surfaces (synthesized through vacuum deposition on a Pt(111) substrate of nonequiatomic Cr-Mn-Fe-Co-Ni or Mn-Fe-Co-Ni alloy (111) lattice stacking layers, followed by a surface Pt(111) layer) depend upon the alloy composition and synthesis temperature: the model catalyst surfaces synthesized with specific combinations of these two parameters outperformed benchmark surfaces such as Pt/equiatomic Cr-Mn-Fe-Co-Ni/Pt(111) in terms of the ORR durability during potential-cycle loading. The outstanding ORR properties are attributed to the use of machine learning to predict synthesis conditions that are closely linked to the atomic-level surface microstructures that favor enhanced ORR properties. These microstructures enable the formation of a so-called "pseudo-core-shell-like structure", i.e., surface Pt(111) underlaid with CCA(111) lattice stacking layers with atomically distributed active elements (Co and/or Ni) close to the surface that are beneficial for ORR property enhancements. This study demonstrates that not only the "high-entropy" effect of charged less-noble CCA elements but also the precise control of elemental distributions in the near-surface vicinity in the pristine state, resulting from optimized CCA compositions and synthesis temperatures, are the key factors to improve Pt-CCA catalyst material systems.
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