通过CO2的三元共价有机框架来详细调节中间体的结合强度,减少反应反应2
Minghao Liu1,2, Cheng-Xing Cui3, Shuai Yang1
1CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute (SARI), Chinese Academy of Sciences (CAS), Shanghai, 201210, P. R. China.
Angewandte Chemie (International ed. in English)
|February 26, 2024
概括
一个新的三组分共价有机框架 (COF) 精确地调节中间结合,以提高电催化CO2的减少. 这种D-AA COF实现了97.2%的法拉第效率,超过了传统的两组合COF.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 电催化二氧化碳还原反应 (CO2RR) 的效率受到中间结合强度的限制.
- 共价有机框架 (COF) 通过捐赠-接受 (DA) 系统提供可调节的结合,但单单元 DA COF 缺乏精确的中间相互作用控制.
- 对于高效的CO2RR催化剂,需要先进的COF设计.
研究的目的:
- 设计和合成一个新的三组合COF与D-A-A单元,以改善CO2RR.
- 调查多组件设计对电子导电性,可还原性和电荷转移的影响.
- 了解在催化部位的中间体的结合相互作用,以提高CO2RR性能.
主要方法:
- 合成一种三组合的COF,其中包括迪亚里胺 (捐赠者),西醇 (接受者) 和Co-porphyrin单位.
- 电催化CO2RR性能评估,包括法拉第效率和部分电流密度测量.
- 分析中间结合能和催化机制的理论计算.
主要成果:
- 与二组件COF相比,三组件COF表现出优越的电子导电性,可还原性和电荷转移.
- 在 -0.8 V 时达到 97.2% 的高法拉代效率,在 -1.0 V 时达到 27.85 mA cm-2 的部分电流密度.
- 理论计算证实了*COOH中间体的最佳结合和*高效的*CO溶解.
结论:
- D-A-A结构的三组件COF有效调节中介结合,以获得更高的CO2RR.
- 这种多元组件策略增强了电荷转移和催化活性,优于传统的DA COF.
- 为设计先进的COF提供了一条途径,以实现高效的CO2转化.
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