是否Fe是Fe/N-Doped Graphdiyne最活跃的部位?
Yuanyi Feng1, Mingying Sun1, Yongfei Ji2
1School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, P. R. China.
ACS omega
|April 22, 2024
概括
用添加的石墨 (GDY) 显示出增强的氧降解反应 (ORR) 活性,这是由于最佳的中间结合. 在GDY中铁和的配合也通过调整结合强度来提高ORR性能.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 纯原石墨丁 (GDY) 由于中介结合较弱,对氧降解反应 (ORR) 的活性有限.
- 优化催化剂活性位点对于高效的ORR催化是至关重要的.
研究的目的:
- 系统地研究原始的ORR活动,Fe-doped,N-doped和Fe/N-codopedGDY.
- 了解兴奋剂对影响ORR活动的电子和几何性质的作用.
主要方法:
- 密度函数理论 (DFT) 的计算.
- 对反应中间体的结合能量的分析.
- 机器学习分析 ΔG ((OH*).
- 调整关系分析和火山情节构建.
主要成果:
- 经过N-兴奋剂的GDY显示出增强的ORR活性,由于中介结合的改善,其低超电位为0.45V.
- 用Fe合的GDY表现出0.43V的超电位,其中最活跃的位点远离Fe.
- Fe/N 编码的 GDY 在 C 位点表现出最佳的活性,与剂保持最佳距离.
- OH*的结合能用作Fe和/或N-doped GDY活动的描述符.
结论:
- 活跃中心及其环境的电子和几何特性显著影响ORR活动.
- 铁和兴奋剂调节中间结合,而最优结合的C位是最活跃的.
- 石墨烯衍生物为高效的ORR电催化剂提供可调节的平台.
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