通过双向协调减少氧的双向协调,急剧扩大单原子分散的Fe-N活性位点
Huihui Jin1,2,3, Ruohan Yu4, Pengxia Ji4
1National Engineering Laboratory for Fiber Optic Sensing Technology, Wuhan University of Technology Wuhan 430070 China zhyli@whut.edu.cn.
Chemical science
|May 17, 2024
概括
兴奋剂增强铁 (Fe-N) 位点,以进行高效的氧降解反应 (ORR). 这项研究引入了一种防止铁聚合的方法,显著提高Fe-N位点密度和Fe-P-NC催化剂中的ORR活性.
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:
- 高密度Fe-N位点对于高效的氧降解反应 (ORR) 是至关重要的.
- 兴奋剂可以降低ORR能量屏障,特别是通过Fe-P键.
- 在高温合成期间的Fe原子聚合阻碍了同时的Fe-P结合和高Fe-N位点密度.
研究的目的:
- 开发一种策略,以防止在高温碳化过程中Fe聚合.
- 在Fe-NC催化剂中实现同时高密度Fe-N位点和Fe-P键.
- 为了增强Fe基催化剂的氧降解反应 (ORR) 活性.
主要方法:
- 使用trifenylphosphine和2-methylimidazole进行双向协调,以限制Fe的生长.
- 合成Fe-P-NC催化剂通过Fe在Fe-NC系统中的酸化.
- 描述催化剂结构并量化单原子分散的Fe位点.
- 执行理论计算以了解反应机制.
主要成果:
- 单原子分散的Fe位点显著增加,从2.8% (Fe-NC) 增加到65.3% (Fe-P-NC).
- 在Fe-P-NC的酸性和性电解质中大大提高了ORR活性.
- 理论计算证实Fe2P促进了Fe-N4位点的中间吸附和电子转移.
- 由于Fe-P键和Fe-N位点的协同效应,减少了反应能量屏障.
结论:
- 双向协调战略有效地防止了Fe聚合,使高密度Fe-N位点和Fe-P键的同时形成成为可能.
- 由此产生的Fe-P-NC催化剂显著提高了ORR性能.
- 这项研究为设计具有更好的活性和稳定性的先进单原子催化剂提供了一条途径.
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