合约Fe-N5-C11 在单原子催化剂中的位置提高了氧降低反应的催化性能
Chao Xu1, Yan-Ping Zhang2, Tian-Long Zheng3
1Key Laboratory for Advanced Materials, School of Chemistry & Molecular Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China.
研究人员开发了新的Fe-N-C单原子催化剂 (SAC),具有独特的可缩小Fe-N5-C11活性位点. 这些催化剂显著提高了能量转换装置中的氧降解反应 (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:
- 在能量转换设备中优化氧降解反应 (ORR) 催化剂性能至关重要.
- 对催化活性位点的控制操作是开发高性能催化剂的关键挑战.
- 单原子催化剂 (SACs) 提供高效率,但需要精确控制活性部位结构.
研究的目的:
- 研究Fe-N5活性位结构对ORR催化活性的影响.
- 开发具有工程,可缩小Fe-N5-C11活性位点的Fe-N-C SAC.
- 为了证明使用这些新型催化剂的能量转换装置的增强性能.
主要方法:
- 合成Fe-N-C SACs使用轴向-意米达-协调铁冠状素前体.
- 使用X射线吸收光谱学 (XAS) 进行表征,以分析活性部位结构和氧化状态.
- 在Zn-空气电池中进行电化学测试和密度函数理论 (DFT) 计算,以评估催化活性和机制.
主要成果:
- 与Fe-N5-C12对应物 (E1/2 = 0.81 V) 相比,Fe-N5-C11催化剂 (C@PVI-(TPC) Fe-800表现出更高的ORR活性 (E1/2 = 0.89 V).
- 这种新型催化剂在气电池中显示出更高的峰值功率密度 (129 mW/cm2).
- XAS揭示了收缩的Fe-N5-C11结构和更高的铁氧化状态,而DFT显示了增加的电子捐赠能力和增强的O2吸附/激活.
结论:
- 工程设计,可缩小的Fe-N5-C11活性位点显著提高ORR催化剂的性能.
- 来自铁的SAC为设计用于能源转换的先进催化剂提供了有希望的途径.
- 这项工作为调整SAC活性站点结构以提高催化剂效率提供了新的策略.
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