基于共价有机框架的单原子催化剂的合理设计,用于氧气演变反应和氧气减少反应
Wenli Xie1, Bin Cui2, Desheng Liu2
1School of Materials Science and Engineering, Guangdong Ocean University, Yangjiang 529500, China.
Molecules (Basel, Switzerland)
|April 26, 2025
概括
基于共价有机框架 (COFs) 的高性能单原子催化剂 (SACs) 对氧演化 (OER) 和氧减少 (ORR) 反应具有前景. Rh/TQBQ和Au/TQBQ表现出极好的催化活性,为清洁能源技术提供了新的设计策略.
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
- 计算化学计算化学
背景情况:
- 对于燃料电池和金属空气电池等可再生能源技术来说,开发高效的氧化演化 (OER) 和氧化减少 (ORR) 催化剂至关重要.
- 两维共价有机框架 (2D COF) 提供了独特的空心位置,非常适合定过渡金属原子,从而创造出有前途的单原子催化剂 (SAC).
研究的目的:
- 系统地调查由TQBQ-COFs支持的SACs的OER和ORR催化性能.
- 了解协调环境对催化活动的影响.
- 为了确定设计高性能SAC的有效描述符.
主要方法:
- 密度函数理论 (DFT) 的计算被用来研究一系列基于TQBQ-COFs的SACs.
- 评估了OER和ORR的催化性能.
- 分析了协调环境和吸附能量的作用.
主要成果:
- Rh/TQBQ表现出最有效的OER性能,其低超电位为0.34V.
- Au/TQBQ表现出优异的ORR性能,其超电位为0.50V.
- 发现TQBQ中的边界氧原子能够独特地影响反应路径,绕过传统的缩放关系.
结论:
- 协调环境对OER和ORR的催化剂性能产生重大影响.
- 过渡金属原子的吸附能 (Ead) 作为预测催化活性的可靠描述器.
- 这项工作为OER/ORR应用设计新的,高效的基于COF的SAC提供了一种新方法.
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