电化学CO2降低过程中的电离体竞争实验作为薄膜改性铜微环境的探测
Madeline H Hicks1, Nicholas B Watkins1, Sebastian Castro1
1Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States.
金属离子会影响电化学二氧化碳减排 (CO2R). 铜电极上的有机薄膜改变了二氧化碳和二氧化碳的传输,通过破坏界面水结构来提高二氧化碳的选择性,而不是通过改变阴离子积累.
科学领域:
- 电化学
- 表面科学
- 催化剂
背景情况:
- 金属离子对电化学二氧化碳减排 (CO2R) 产品的选择性和活性产生重大影响.
- 子影响CO2R的确切机制尚未完全阐明.
- 了解这些机制对于设计高效的CO2R催化剂至关重要.
研究的目的:
- 在二氧化碳中解构离子依赖的电场和非电场效应
- 研究有机薄膜改性铜电极在调节阴离子影响中的作用.
- 阐明改善CO2R选择性的机制途径.
主要方法:
- 使用LiHCO3和CsHCO3进行的阳离子竞争实验.
- 在裸体和有机薄膜改性Cu电极上进行电化学CO2降低 (CO2R).
- 用于现场分析的减弱全反射表面增强红外吸收光谱 (ATR-SEIRAS).
主要成果:
- 有机添加剂薄膜不会改变电化学界面的积累.
- 薄膜改变了CO2和CO传输和界面度,减少了增强CO2R所需的Cs+.
- 离子 (Cs+) 破坏水界结构,促进CO2R转化为CO和C-C合产物.
结论:
- 光谱证据证实有机薄膜改性电极增强了CO2R的选择性.
- 这项研究将二氧化碳中的电场和非电场离子效应脱.
- 通过阴离子对水的界面结构进行修改是促进CO2R的关键.
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