通过增加累积的带电中间体和促进的*CO二聚变,NHC-CDI联体促进了电催化CO2的多碳生产
Kirstine Nygaard Kolding1,2, Matias Bretlau2, Siqi Zhao2,3
1Carbon Dioxide Activation Center (CADIAC), Interdisciplinary Nanoscience Center (iNANO), Aarhus University, 8000 Aarhus C, Denmark.
Journal of the American Chemical Society
|May 3, 2024
概括
分子功能化铜催化剂显著提高了二氧化碳减少的多碳产品的形成. 受到分子添加剂影响的表面电荷积累是增强有价值碳化合物的催化活性和选择性的关键.
科学领域:
- 电化学
- 材料科学
- 催化剂
背景情况:
- 基于铜的材料是电化学二氧化碳 (CO2) 减少的有希望的催化剂,特别是用于产生多碳化合物.
- 铜电极的分子功能化提供了一种通过定制表面微环境来增强催化活性的策略.
- 有限的机械学理解往往阻碍了表面修饰剂在二氧化碳电减中的作用的确确定.
研究的目的:
- 调查N-异环碳胺功能化铜催化剂对二氧化碳的降低效率.
- 阐明分子添加剂和表面电荷在促进多碳产品形成中的机械作用.
- 使用气体扩散电极电解器实现高选择性和部分电流密度的多碳产品.
主要方法:
- 合成和表征N- heterocyclic carbene-carbodiimide功能化的铜催化剂.
- 使用气体扩散电极电解器进行电化学二氧化碳减排实验.
- 使用X射线光电子光谱 (XPS) 和现场拉曼光谱进行表面分析.
主要成果:
- 与纯铜相比,功能化铜催化剂在多碳产品形成方面表现出一个数量级更高的活性.
- 对于部分电流密度约为-80 mA cm-2的多碳产品,获得了58%的选择性.
- 鉴定了由于中间积累的表面电荷积累作为活性的一个关键因素,分子添加剂稳定了表面CO并促进了Cu步位的C-C合.
结论:
- 分子表面改造是开发有效的二氧化碳减排电催化剂的有效策略.
- 表面电荷在决定多碳产物形成活动方面起着至关重要的作用.
- 了解中间稳定和结合点对于设计先进的二氧化碳减排催化剂至关重要.
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