在电化学CO2降低过程中,Ag催化剂表面的化学修饰用Imidazolium Ionomers调节H2进化率
David M Koshy1,2, Sneha A Akhade3, Adam Shugar1
1Department of Chemical Engineering, Stanford University, Stanford, California 94305 United States.
Journal of the American Chemical Society
|September 2, 2021
概括
在白银催化剂上,伊米达离子体并没有增强二氧化碳降解到二氧化碳,但显著促进了的演变. 离子体结构上的体质量限制了这种的进化,为电化学反应器提供了设计见解.
科学领域:
- 电化学
- 材料科学
- 催化剂
背景情况:
- 优化电化学反应器对于能源和可持续性至关重要.
- 聚合物设计和催化剂表面科学相互作用可以调整反应器的性能.
- 有机-无机接口影响反应的选择性和活性.
研究的目的:
- 调查基于伊米达的离子体在银表面的电催化二氧化碳 (CO2R) 降解中的作用.
- 了解离子体如何影响CO2R和竞争的演化反应 (HER).
- 确定离子体结构对催化活性的影响.
主要方法:
- 测量CO2R和HER速率的电催化实验
- 基于变化的二氧化碳和二氧化碳 (HCO3-) 度的动态建模.
- 使用塔夫特硬质参数对离子体结构-活性关系的分析.
- 密度函数理论 (DFT) 的计算.
主要成果:
- 伊米达离子对Ag表面的CO2R活性没有影响.
- 对于竞争对手的 HER,
- 动态建模表明通过离子体对HCO3降解的内在促进.
- 不同的离子体结构调节了HER的提升,而硬质体量则限制了这种效果.
结论:
- 离子体结构中的固体阻碍限制了与催化剂表面和基板的相互作用.
- 这些发现为CO2R中的离子体-催化剂相互作用提供了设计规则.
- 需要进一步研究以了解电催化中的协调效应.
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