Assessing factors that determine adatom migration and clustering on a thin film oxide; Pt1 and Rh1 on the “29” CuxO/Cu(1 1 1) surface
Assessing factors that determine adatom migration and clustering on a thin film oxide; Pt1 and Rh1 on the “29” CuxO/Cu(1 1 1) surface
复制标题
评估决定吸附原子在薄膜氧化物上迁移和聚集的因素；
DOI：
10.1016/j.apsusc.2023.157145
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发表时间：
2023
影响因子：
6.7
通讯作者：
McEwen, Jean-Sabin
中科院分区：
文献类型：
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作者：
Ulumuddin, Nisa;Çınar, Volkan;Schilling, Alex C.;Hunt, Adrian;Waluyo, Iradwikanari;Sykes, E. Charles;McEwen, Jean-Sabin
单活性中心催化剂在非平衡条件下的动力学性质对其活性中心的全面表征提出了重大挑战。“29”氧化物是在Cu（111）上生长的薄CuxO膜，其提供了良好限定的表面，在该表面上研究原子分散的贵金属的结构和化学。结合实验和第一性原理的方法被用来研究影响金属吸附原子的流动性和他们的集群趋势的因素。我们的工作阐明了如何一个均匀的协调环境中性单原子时，它的倾向，以打破其附近的氧化物键是低的，可以获得。我们证明，这反过来又会影响薄膜氧化物上原子分散的物种的化学活性，因为氧化物上的缺陷实际上会使这些物种更容易接触到CO。因此，我们强调了理解缺陷和原子分散的活性位点之间的关系的重要性设计单位点催化剂。
The dynamical nature of single-site catalysts under non-equilibrium conditions poses significant challenges in the full characterization of their active sites. The “29” oxide is a thin CuxO film grown on Cu(1 1 1) which provides a well-defined surface on which to study the structure and chemistry of atomically dispersed precious metals. A combination of experimental and first-principles approaches is used to investigate the factors that influence the mobility of metal adatoms and their clustering tendencies. Our work elucidates how a homogenous coordination environment of neutral single-atoms can be obtained when its tendency to break oxide bonds within its vicinity is low. We demonstrate that this in turn affects the chemical activity of atomically dispersed species on thin-film oxides, as defects on the oxide would in fact allow such species to be more accessible to CO. We thus highlight the importance of understanding the relationship between defects and atomically dispersed active sites upon designing single-site catalysts.