Defective NiO as a Stabilizer for Au Single-Atom Catalysts
Defective NiO as a Stabilizer for Au Single-Atom Catalysts
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DOI：
10.1021/acscatal.2c00108
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发表时间：
2022-05
期刊：
影响因子：
12.9
通讯作者：
C. Mochizuki;Yusuke Inomata;Shunsaku Yasumura;Mingyue Lin;Ayako Taketoshi;T. Honma;N. Sakaguchi;M. Haruta;K. Shimizu;T. Ishida;T. Murayama
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文献类型：
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作者：
C. Mochizuki;Yusuke Inomata;Shunsaku Yasumura;Mingyue Lin;Ayako Taketoshi;T. Honma;N. Sakaguchi;M. Haruta;K. Shimizu;T. Ishida;T. Murayama
单原子催化剂由于其不同于纳米颗粒催化剂的电子和结构性质而显示出突出的催化活性。然而，对于Au单原子催化剂，能够稳定单原子状态的金属氧化物仍然有限，并且稳定效果还不为人所知。在这里，我们报告Au单原子催化剂负载在NiO（Au 1/NiO），其结构特征，和它们的催化性能。Au原子分散在具有Ni空位的NiO表面。与清洁的NiO表面相比，在具有Ni空位的NiO表面上更有利于Au单原子位点的形成。Au单原子是阳离子，其电荷状态取决于晶面[NiO（100）上的Au 3 +-like; NiO（110）上的Au+-like]。在室温下，0.011wt%Au 1/NiO催化剂对CO氧化的周转频率（0.41 s-1）高于NiO负载纳米颗粒Au催化剂的周转频率（0.033 s-1）. Au 1/NiO对CO氧化反应表现出很高的催化稳定性（120 °C，120 h）。
Single-atom catalysts show outstanding catalytic activity owing to their different electronic and structural properties from those of nanoparticulate catalysts. For Au single-atom catalysts, however, metal oxides that can stabilize a single atomic state are still limited and the stabilizing effect is not well known. Here, we report Au single-atom catalysts supported on NiO (Au1/NiO), their structural features, and their catalytic properties. Atomic Au was dispersed on the surface of NiO with Ni vacancy sites. The formation of Au single-atom sites was more favorable on an NiO surface with Ni vacancy sites than on a clean NiO surface. The Au single atoms were cationic, and their charge states depended on the crystal facets [Au3+-like on NiO(100); Au+-like on NiO(110)]. The turnover frequency (TOF) of 0.011 wt % Au1/NiO for CO oxidation (0.41 s–1) was higher than the TOFs of nanoparticulate Au catalysts supported on NiO (0.033 s–1) at room temperature. Au1/NiO showed a high catalytic stability (120 °C, 120 h) to CO oxidation reaction.