期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 22, 期 7, 页码 3983-3989出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cp05349b
关键词
-
资金
- National Natural Science Foundation of China [91545122]
- Beijing Natural Science Foundation [2182066]
- Natural Science Foundation of Hebei Province of China [B2018502067]
- University of Calgary's Canada First Research Excellence Fund (CFREF) program entitled the Global Research Initiative for Sustainable Low Carbon Unconventional Resources
The stability of a single-atom catalyst is directly related to its preparation and applications, especially for high-loading single-atom catalysts. Here, the effect of a coordination environment induced by nitrogen (N) atoms coordinated with iron on the kinetic and thermodynamic stabilities of single-atom iron catalysts supported with carbon-based substrates (Fe-SA/CS) was investigated by density functional theory (DFT) calculations. Five Fe-SA/CS with different numbers of N atoms were modelled. The kinetic stability was evaluated by analyzing the migration paths of iron atoms and energy barriers. The thermodynamic stability was studied by calculating the adsorption and formation energies. Our results indicated that the coordination environment induced by N can promote the kinetic and thermodynamic stability of Fe-SA/CS. N atoms on the substrate promote the kinetic stability by raising the energy barrier for iron migration and not only increase the thermodynamic stability, but also contribute to catalyst synthesis. Doping N on the substrate enhances charge transfer between the iron atoms and substrates simultaneously improving the kinetic and thermodynamic stabilities. This theoretical research provides guidance for synthesizing stable and high loading single-atom catalysts by tuning the coordination environment of single-atom elements.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据