College of Materials Science and Engineering, China Jiliang University, Hangzhou 310018, China.
Nanoscale. 2019 Mar 14;11(11):5064-5071. doi: 10.1039/c8nr09300h.
Although single metal atoms (SMAs) have been extensively investigated as unique active sites in single-atom catalysts, the possible active sites of the host catalysts have been unfortunately neglected in previous studies. In single-atom catalysts, the SMAs can promote the chemical and catalytic activities of host atoms, which may act as secondary active sites, resulting in a significant synergistic effect on the catalytic performance. Using density functional theory calculations, we studied the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) on two different types of active sites: single metal (M1) atoms and the neighboring host atoms of several M1/g-C3N4 samples. The contributions of M1 and host atoms towards the reduction of the OER/ORR overpotentials of Fe1, Co1, Ni1, Cu1 and Zn1/g-C3N4, bifunctional electrocatalysts with the OER/ORR overpotentials of 0.50-0.70 V were investigated. Finally, new M1/g-C3N4 catalysts with high OER/ORR performances could be estimated based on the d-band centre of the M1 atoms in the future.
虽然单金属原子（SMAs）作为单原子催化剂中的独特活性位点已经得到了广泛的研究，但在以前的研究中，宿主催化剂的可能活性位点却不幸被忽视了。在单原子催化剂中，SMAs 可以促进宿主原子的化学和催化活性，这些原子可能充当次级活性位点，从而对催化性能产生显著的协同效应。我们使用密度泛函理论计算，研究了两种不同类型的活性位点上的氧气析出反应（OER）和氧气还原反应（ORR）：单金属（M1）原子和几种 M1/g-C3N4 样品中 M1 近邻的宿主原子。我们研究了 M1 和宿主原子对 Fe1、Co1、Ni1、Cu1 和 Zn1/g-C3N4 的 OER/ORR 过电势降低的贡献，这些双功能电催化剂的 OER/ORR 过电势为 0.50-0.70V。最后，未来可以根据 M1 原子在 d 带中心的位置来估计具有高 OER/ORR 性能的新型 M1/g-C3N4 催化剂。
