Atom(片上系统)
材料科学
密度泛函理论
催化作用
金属
纳米技术
化学物理
联轴节(管道)
碳纤维
计算化学
计算机科学
化学
复合材料
复合数
冶金
嵌入式系统
生物化学
作者
Kevin Rossi,Andrea Ruiz‐Ferrando,Dario Faust Akl,Victor Gimenez Abalos,Javier Heras‐Domingo,Romain Graux,Xiao Hai,Jiong Lu,Dario Garcia‐Gasulla,Núria López,Javier Pérez‐Ramírez,Sharon Mitchell
标识
DOI:10.1002/adma.202307991
摘要
Abstract Ultra‐high‐density single‐atom catalysts (UHD‐SACs) present unique opportunities for harnessing cooperative effects between neighboring metal centers. However, the lack of tools to establish correlations between the density, types, and arrangements of isolated metal atoms and the support surface properties hinders efforts to engineer advanced material architectures. Here, this work precisely describes the metal center organization in various mono‐ and multimetallic UHD‑SACs based on nitrogen‐doped carbon (NC) supports by coupling transmission electron microscopy with tailored machine‐learning methods (released as a user‐friendly web app) and density functional theory simulations. This approach quantifies the non‐negligible presence of multimers with increasing atom density, characterizes the size and shape of these low‑nuclearity clusters, and identifies surface atom density criteria to ensure isolation. Further, it provides previously inaccessible experimental insights into coordination site arrangements in the NC host, uncovering a repulsive interaction that influences the disordered distribution of metal centers in UHD‐SACs. This observation holds in multimetallic systems, where chemically‐specific analysis quantifies the degree of intermixing. These fundamental insights into the materials chemistry of single‐atom catalysts are crucial for designing catalytic systems with superior reactivity.
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