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  11. 金属-有机框架 选择性co2电减调节

金属-有机框架 选择性CO2电减调节

Dae-Hyun Nam1, Oleksandr S Bushuyev1, Jun Li1,2

  • 1Department of Electrical and Computer Engineering , University of Toronto , 10 King's College Road , Toronto , Ontario M5S 3G4 , Canada.

Journal of the American Chemical Society
|August 17, 2018

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在PubMed 上查看摘要

概括
此摘要是机器生成的。

研究人员开发了一种使用金属有机框架 (MOF) 创建铜 (Cu) 集群的新方法. 这种策略增强了电化学二氧化碳减排反应 (CO2RR),用于生产有价值的多碳产品,如乙烯.

科学领域:

  • 材料科学
  • 电化学
  • 催化剂

背景情况:

  • 电化学二氧化碳还原反应 (CO2RR) 对于将二氧化碳转化为有价值的化学物质至关重要.
  • 铜 (Cu) 集群是CO2RR的有希望的催化剂,但控制它们的选择性,特别是对于多碳产品,仍然具有挑战性.
  • Cu活性位点的表面协调数 (CN) 显著影响CO2RR结果.

研究的目的:

  • 通过金属有机框架 (MOF) 制定规范Cu集群形成的策略,以提高CO2RR向多碳产品.
  • 通过控制聚物的前体结构来促进缺乏协调的位.
  • 在Cu集群CN和CO2RR选择性之间建立结构-活动关系.

主要方法:

  • 使用HKUST-1,一个金属有机框架 (MOF),作为Cu集群形成的模板.
  • 用热处理的HKUST-1将对称的立方体扭曲成不对称的图案,从而产生低协调的位点.
  • 使用电子磁共振 (EPR) 和现场X射线吸收光谱 (XAS) 来描述Cu星团及其电子状态.
  • 研究了不同材料加工条件对立体结构和CO2RR性能的影响.

主要成果:

  • 从HKUST-1中的扭曲Cu二元中成功促进了低协调数 (CN) 的Cu集群的形成.
  • 使用这些MOF衍生的Cu聚合催化剂,实现了C2H4 (乙烯) 生产的创纪录的45%法拉达效率 (FE).
  • 证明调节 Cu-Cu CN 在 Cu 集群是控制 CO2RR 选择性的关键.

结论:

  • MOF规范的合成策略有效地控制了Cu集群的形成,并促进了缺乏协调的活跃地点.
  • 这种方法提供了一种选择性地从二氧化碳电解产生多碳产品的途径.
  • 已建立的结构-活动关系为设计CO2RR的先进Cu催化剂提供了洞察力.

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