Rao Yi, Wu Yutong, Dai Xueya, Zhang Ya-Wen, Qin Gaowu, Qi Wei, Li Song
Key Lab for Anisotropy and Texture of Materials (MoE), School of Materials Science and Engineering, Northeastern University, Shenyang, 110819, P. R. China.
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, P. R. China.
Small. 2022 Dec;18(51):e2204611. doi: 10.1002/smll.202204611. Epub 2022 Oct 18.
Single-atom catalysts (SACs) exhibit distinct catalytic behavior compared with nano-catalysts because of their unique atomic coordination environment without the direct bonding between identical metal centers. How these single atom sites interact with each other and influence the catalytic performance remains unveiled as designing densely populated but stable SACs is still an enormous challenge to date. Here, a fabrication strategy for embedding high areal density single-atom Pt sites via a defect engineering approach is demonstrated. Similar to the synergistic mechanism in binuclear homogeneous catalysts, from both experimental and theoretical results, it is proved that electrons would redistribute between the two oxo-bridged paired Pt sites after hydrogen adsorption on one site, which enables the other Pt site to have high CO oxidation activity at mild-temperature. The dynamic electronic interaction between neighboring Pt sites is found to be distance dependent. These new SACs with abundant Pt-O-Pt paired structures can improve the efficiency of CO chemical purification.
单原子催化剂（SACs）由于其独特的原子配位环境，且相同金属中心之间没有直接键合，因此与纳米催化剂相比表现出独特的催化行为。由于设计高密度但稳定的单原子催化剂至今仍是一个巨大的挑战，这些单原子位点如何相互作用并影响催化性能仍不为人知。在此，展示了一种通过缺陷工程方法嵌入高面密度单原子铂位点的制备策略。与双核均相催化剂中的协同机制类似，从实验和理论结果都证明，在一个位点上吸附氢后，电子会在两个氧桥联配对的铂位点之间重新分布，这使得另一个铂位点在温和温度下具有高的一氧化碳氧化活性。发现相邻铂位点之间的动态电子相互作用与距离有关。这些具有丰富Pt-O-Pt配对结构的新型单原子催化剂可以提高一氧化碳化学净化的效率。
