Zheng Tao, Han Xiao, Wang Jincheng, Xia Zhenhai
State Key Laboratory of Solidification Processing, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an, 710072, P.R. China.
Department of Materials Science and Engineering, University of North Texas, Denton, TX 76203, USA.
Nanoscale. 2022 Nov 10;14(43):16286-16294. doi: 10.1039/d2nr04880a.
Single-atom catalysts (SACs) are promising as efficient electrocatalysts for clean energy technologies such as fuel cells, water splitting, and metal-air batteries. Still, the unsatisfactory loading density and stability of the catalytic active centers limit their applications. Herein, a doping strategy is explored to achieve highly efficient and stable SACs for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The stability, electronic structures, and ORR/OER overpotentials of S-doped transition metal-nitrogen-carbon SAC structures were investigated using first-principles calculation methods. An intrinsic descriptor linking the intrinsic properties of catalysts and the catalytic activity was established for screening the best SACs. The theoretical predictions are well consistent with the experimental results, which provide a theoretical basis for understanding the catalytic mechanism and an approach for the rational design of SACs for clean energy conversion and storage.
单原子催化剂（SACs）作为用于燃料电池、水分解和金属空气电池等清洁能源技术的高效电催化剂具有广阔前景。然而，催化活性中心的负载密度和稳定性不尽人意限制了它们的应用。在此，探索了一种掺杂策略以实现用于氧还原反应（ORR）和析氧反应（OER）的高效且稳定的SACs。使用第一性原理计算方法研究了S掺杂的过渡金属氮碳SAC结构的稳定性、电子结构以及ORR/OER过电位。建立了一个将催化剂的内在性质与催化活性联系起来的本征描述符，用于筛选最佳的SACs。理论预测与实验结果高度一致，这为理解催化机理提供了理论基础，并为合理设计用于清洁能源转换和存储的SACs提供了一种方法。
