通过对界面Cu-O键的强度进行工程,改变CO2电还原通路到C1或C2+产品
Yu Zhang1, Yicheng Li1, Nana Gao2
1School of Mechanical and Power Engineering, East China University of Science and Technology, 130 Meilong Road, 200237, Shanghai, China.
Angewandte Chemie (International ed. in English)
|June 16, 2024
概括
优化铜催化剂与有机物种的协调可以合理地改变电催化二氧化碳减排 (CO2RR) 途径. 这项研究指导了用于选择性C1或C2+产品生成的基于Cu的催化剂的设计,从而促进了CO2利用.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 基于铜 (Cu) 的催化剂对于将二氧化碳 (CO2) 转化为有价值产品至关重要.
- 电催化二氧化碳减排反应 (CO2RR) 为二氧化碳利用提供了一个有前途的途径.
- 控制CO2RR对特定产品 (C1与C2+) 的选择性仍然是一个重大挑战.
研究的目的:
- 为了证明如何优化Cu与含有O的有机物种 (二氧化酸和环素) 的协调,可以合理地改变CO2RR路径.
- 研究Cu-O键强度对催化剂形态,电子结构和CO2RR性能的影响.
- 为选择性二氧化碳转化提供基于Cu的催化剂的合理设计提供见解.
主要方法:
- 与酸 (C4O4-Cu) 和环素 (C6O6-Cu) 协调的基于Cu的催化剂的合成.
- 电催化二氧化碳还原反应 (CO2RR) 测量以评估产品选择性和法拉第效率 (FE).
- 催化剂形态和电子结构的表征与催化性能相关联.
主要成果:
- 具有有组织的纳米领域的C6O6-Cu催化剂主要产生C1产品,FE在-0.6V时为63.7%,而RHE为63.7%.
- 具有近乎完美的晶体结构和均分散的Cu原子的C4O4-Cu催化剂,在C2+产品中达到65.8%的FE,表明增强了C-C合.
- C4O4-Cu系统在205.1mA/cm2的高电流密度下,在-1.0V与RHE相比,在10个多小时内表现出稳定的运行.
结论:
- 与含有氧的有机物种的协调环境是指导CO2RR选择性的关键因素.
- 调节Cu-O键强度会影响催化剂结构和电子特性,从而可以控制C1与C2+产品的形成.
- 本研究提供了一个合理的设计策略,用于开发高效和选择性的基于Cu的电催化剂,用于二氧化碳转化,接近实际相关性.
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