富含环氧元素的Fe单原子站点 增加氧气 减少 电催化 电催化
Yufei Zhao1, Ziyan Shen1, Juanjuan Huo1
1Joint International Laboratory on Environmental and Energy Frontier Materials, School of Environmental and Chemical Engineering, Shanghai University, China.
Angewandte Chemie (International ed. in English)
|July 15, 2023
概括
新的单原子催化剂具有铁与硫和氧组 (Fe1/NSOC) 显著提高氧降解反应效率. 这一突破为能源设备中贵金属催化剂提供了一个有希望的,高效的替代品.
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:
- 电催化剂对于高效的能量转换和储存至关重要.
- 单原子催化剂提供优越的金属利用率和可调节的电子性能,为贵金属提供了替代品.
- 了解不同物种在单原子催化剂中固定点的精确作用仍然是一个挑战.
研究的目的:
- 开发和研究新型的铁单原子催化剂 (Fe1/NSOC),其中包含硫和氧的功能组,以提高氧降解反应 (ORR) 的性能.
- 阐明负责改善催化活性的原子层机制.
主要方法:
- 用硫和氧功能组 (Fe1/NSOC) 合成Fe单原子催化剂.
- 电化学表征,包括半波电位测量.
- 用光谱分析探测催化剂的电子结构和组成.
- 密度函数理论 (DFT) 计算以建模催化机制.
主要成果:
- Fe1/NSOC实现了0.92V的高半波潜力与RHE相比,在添加碳 (Fe1/NC) 上表现优于商业Pt/C和Fe单原子催化剂.
- 光谱数据表明,硫基在FeN4S2中心附近诱导环氧基,调节铁的电子结构.
- DFT的计算证实,硫和环氧基优化了Fe活性位点的电荷,并促进了速率限制步骤 (OH*去除).
结论:
- 与现有基准相比,Fe1/NSOC显示出更高的ORR电催化活性.
- 硫和环氧基的协同作用对于增强铁单原子催化剂的电子特性和催化动力学至关重要.
- 这项工作为高效非贵金属电催化剂的设计原则提供了基本的见解.
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