Understanding the Activity of Single-Atom Catalysis from Frontier Orbitals
Understanding the Activity of Single-Atom Catalysis from Frontier Orbitals
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DOI：
10.1103/physrevlett.125.156001
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发表时间：
2020-10-08
影响因子：
8.6
通讯作者：
Wu, Ruqian
中科院分区：
文献类型：
--
作者：
Fu, Zhaoming;Yang, Bowen;Wu, Ruqian
d 带中心和电荷态通常用于分析贵金属或过渡金属表面和团簇的催化活性，但它们对单原子催化剂 (SAC) 的适用性尚不确定。这项工作表明，最接近 SAC 费米能级的前沿轨道的空间结构和方向起着至关重要的作用。以C3N负载的单原子Au上的多个分子的吸附和CO的氧化为例，我们证明了吸附和催化活性与前线轨道的特征密切相关。这项工作为理解单原子催化剂的性能提供了有效的指导。
The d-band center and charge states are often used to analyze the catalytic activity of noble or transition metal surfaces and clusters, but their applicability for single-atom catalysts (SACs) is unsure. This work suggests that the spatial structure and orientation of frontier orbitals which are closest to the Fermi level of SACs play a vital role. Taking adsorption of several molecules and CO oxidization on C3N-supported single-atom Au as examples, we demonstrate that adsorption and catalytic activities are well correlated with the characteristics of frontier orbitals. This work provides an effective guidance for understanding the performance of single-atom catalysts.