酸性和性pH控制氧降解反应路径在Co-N4C催化剂上
Bikash K Mahapatra1, Pranjit Barman1, Dipti R Panigrahi1
1Department of Chemistry, School of Natural Sciences, Shiv Nadar Institution of Eminence (SNIoE), NH91, Tehsil Dadri, Gautam Buddha Nagar, Greater Noida, Uttar Pradesh, 201314, India.
这项研究引入了一个多孔的单原子催化剂 (pCo-N4C),用于增强氧降解反应 (ORR). 催化剂的动力学与相似,在酸性和性介质中的活性差异是由质子效应解释的.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 氧降解反应 (ORR) 对燃料电池和金属空气电池至关重要.
- 具有M-N4 / C结构的单原子催化剂 (SAC) 对ORR有希望.
- 了解SAC中的pH依赖ORR机制对于设备优化至关重要.
研究的目的:
- 为ORR合成和描述一个多孔的单原子催化剂 (pCo-N4C).
- 研究pCo-N4C在酸性和性电解质中的ORR活性中的机制差异.
- 用计算方法阐明pH对催化性能的作用.
主要方法:
- 在石墨烯框架中,合成一个多孔的单原子催化剂 (pCo-N4C) 与协调到.
- 在0.1m HClO4和0.1m KOH中对ORR的pCo-N4C的电化学评估.
- 基于密度函数理论 (DFT) 计算的ab-initio分子动力学 (AIMD) 模拟.
主要成果:
- 该pCo-N4C催化剂促进了直接的4e-ORR过程,其动力学与Pt/C相竞争.
- 酸性电解质中的较高活性归因于性诱导的疏水性.
- 观察到与质质子和受限质子合电子转移 (PCET) 相关的ORR发起电位 (0.82V在酸中,0.91V在中) 的差异.
结论:
- 合成的pCo-N4C是一种有效的ORR催化剂,其活性可根据pH调节.
- 协调的质子化和受限制的PCET显著影响不同电解质的ORR性能.
- 该研究提供了对SACspH依赖机制的见解,指导了能源应用的未来催化剂设计.
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