挖掘自身位点：线性配位稳定 Pt1/Fe2O3 单原子催化剂
Digging its own Site: Linear Coordination Stabilizes a Pt1/Fe2O3 Single-Atom Catalyst
AI总结：
本研究结合 STM、XPS 与演化计算搜索，揭示 Pt 单原子通过重构 Fe2O3 表面形成稳定的准线性 O—Pt—O 配位。
摘要：
确定活性位点的局部配位是可靠模拟单原子催化剂（SACs）的先决条件。在基于粉末的体系上获得此类信息十分困难，因此大量重点被放在基于载体理想化低指数表面的密度泛函理论计算上。本工作中，我们研究 Pt 原子如何结合到 Fe2O3 的（1-102）晶面，Fe2O3 是 SAC 中常用的载体材料。结合扫描隧道显微镜（STM）、X 射线光电子能谱（XPS）以及广泛的计算演化搜索，我们发现 Pt 原子显著重构载体晶格，以促成与表面氧原子的准线性配位。尽管断裂了三个表面 Fe—O 键，该几何结构仍比涉及未受扰动载体的最佳构型稳定 0.84 eV。我们认为线性 O—Pt—O 构型在反应性 Pt 基 SAC 体系中很常见，因为它在热稳定性与从气相吸附反应物的能力之间取得平衡，并且广泛的结构搜索可能是确定单原子催化中真实活性位点几何结构所必需的。
英文摘要：
Determining the local coordination of the active site is a pre-requisite for the reliable modeling of single-atom catalysts (SACs). Obtaining such information is difficult on powder-based systems, so much emphasis is placed on density functional theory-based computations based on idealized low-index surfaces of the support. In this work, we investigate how Pt atoms bind to the (1-102) facet of Fe2O3, a common support material in SAC. Using a combination of scanning tunneling microscopy (STM), x-ray photoelectron spectroscopy (XPS), and an extensive computational evolutionary search, we find that Pt atoms significantly reconfigure the support lattice to facilitate a pseudo-linear coordination to surface oxygen atoms. Despite breaking three surface Fe-O bonds, this geometry is favored by 0.84 eV over the best configuration involving an unperturbed support. We suggest that the linear O-Pt-O configuration is common in reactive Pt-based SAC systems because it balances thermal stability with the ability to adsorb reactants from the gas phase, and that extensive structural searches are likely necessary to determine realistic active site geometry in single-atom catalysis.
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