对称性依赖的轨道参与控制C2 选择性在CO/CO2 减少M-NxB单原子催化剂
Sourav Ghosh1, Asif Iqbal1, Ranjit Thapa1,2
1Department of Physics, SRM University-AP, Amaravati, Andhra Pradesh 522 240, India.
The journal of physical chemistry letters
|January 9, 2026
概括
具有-邻的单原子催化剂可通过CO2RR有效生产乙烯和乙醇等C2产品. 这一突破克服了二氧化碳减排反应的局限性,为先进的催化方式铺平了道路.
科学领域:
- 催化剂是一种催化剂.
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
背景情况:
- 单原子催化剂 (SAC) 在产生C2产品方面面临限制,原因是缺少双重活性位点和并发演化反应 (HER).
- 现有的SAC在一氧化碳 (CO) 和二氧化碳 (CO2) 减少反应 (CORR/CO2RR) 中努力实现高效的C2选择性.
研究的目的:
- 在CORR和CO2RR中设计和研究具有- (N-B) 邻近的新型SAC,以提高C2产品选择性.
- 确定特定的金属活性中心,并了解控制C2形成的催化机制.
主要方法:
- 28个金属-N-B (MNxB) 单原子催化剂系统的计算选.
- 密度函数理论 (DFT) 计算以确定限制潜力和反应路径.
- 分析电子结构,包括轨道占用率和电子捐赠/反捐赠,以阐明反应机制.
主要成果:
- 确定了Fe,Co,Rh和Ni作为MNxBSAC中的有前途的活性中心,用于C2产品生成.
- 在COR和CO/CO2RR中使用FeN3B实现了0.66V的低限制潜力,用于C2生产.
- 建立了↓d_yz轨道占用率和CO-CO结合能量 (R2 = 0.74) 之间的强烈相关性,解释了CO-CO合机制.
- 提供了对有利于C2产品形成的几何和电子因素 (σ-捐赠,π-回捐赠) 的见解.
结论:
- 具有N-B邻域的SAC有效地克服了以前的限制,在CO的存在下通过CO2RR进行选择性C2生产 (乙烯,乙醇).
- M NxB系统在CORR中显示出C2合成的巨大潜力,扩大了超出铜基催化剂的催化能力.
- 这项工作为设计高效C2电催化剂的先进SAC提供了新的途径.
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