快速CO电还原到和环 (C3+) 的反应机制在三原子催化剂上
Mohsen Tamtaji1, Soonho Kwon2, Charles B Musgrave2
1Hong Kong Quantum AI Lab Limited, Pak Shek Kok, Hong Kong SAR 999077, China.
ACS applied materials & interfaces
|June 26, 2024
概括
具有应力金属中心的三原子催化剂 (TAC) 有效地将一氧化碳 (CO) 转化为有价值的C2+和C3+化学物质. 铁 (Fe3N7) 和 (Ir3N7) 显示出合成低超电位的,环和乙烯的前景.
科学领域:
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
- 电化学 电化学 电化学
背景情况:
- 一氧化碳还原反应 (CORR) 对于将二氧化碳和二氧化碳转化为增值化学品至关重要.
- 生产烯和环烯等C2+和C3+产品可在聚合物和制药领域提供工业应用.
- 现有的催化剂往往缺乏针对性C3+合成所需的效率和选择性.
研究的目的:
- 引入和研究三原子催化剂 (TACs) 以有效减少CO2到C3+产品.
- 使用计算方法选过渡金属,以获得最佳的催化活性,以减少二氧化碳排放.
- 阐明反应机制,并预测关键C2+和C3+产品的过度潜力.
主要方法:
- 使用大规范电位动力学 (GCP-K) 支持配合石墨烯 (M3N7) 的12种过渡金属的计算选.
- 分析CO结合,结合和C-C二元化能量,以确定有希望的催化剂候选者.
- 密度函数理论 (DFT) 的计算用于研究反应机制,并预测Fe3N7和Ir3N7.7的过度潜力.
主要成果:
- Fe3N7和Ir3N7被确定为减少CO2到C3+产品的最佳候选者.
- DFT预测Fe3N7对烯 (0.17V_RHE) 和环烯 (0.42V_RHE) 的低超电位.
- DFT预测在室温和pH7下,Ir3N7对乙烯 (0.15V_RHE) 的过高潜力很低.
结论:
- 三重原子催化剂 (TAC) 提供了一种选择性减少二氧化碳到C2+和C3+产品的新策略.
- Fe3N7和Ir3N7显示出从二氧化碳中合成有价值的有机化学物质的巨大潜力.
- 这项研究为设计用于可持续化学合成的先进电催化剂提供了基本的见解.
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