选择性CO2降解以乙烯通过适应性小分子工程介导的基于铜的电催化剂
Shenghua Chen1, Chengliang Ye2, Ziwei Wang3
1National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology, School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, 710049, P. R. China.
Angewandte Chemie (International ed. in English)
|October 30, 2023
概括
酸修改铜催化剂以有效的电化学减少二氧化碳 (CO2 RR) 到乙烯 (C2H4). 这一战略提高了选择性和产量,克服了二氧化碳转化方面的挑战.
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:
- 使用铜 (Cu) 催化剂的电化学二氧化碳降解 (CO2 RR) 到乙烯 (C2H4) 显示出对二氧化碳转化有希望.
- 在CO2 RR过程中Cu催化剂的结构重建阻碍了高C2H4选择性.
研究的目的:
- 制定一项用于in situ分子修改Cu催化剂的策略,以提高CO2 RR期间的C2H4选择性.
- 研究酸 (TA) 在调节Cu催化剂结构和性能方面的作用.
主要方法:
- 使用酸 (TA) 在位分子修饰.
- 电化学 CO2 减少反应 (CO2 RR) 在流电池中.
- 在现场的X射线吸收光谱 (XAS) 和拉曼光谱.
- 理论计算 (密度函数理论 - DFT).
主要成果:
- 在高电流密度 (497.2 mA cm-2) 的C2H4中使用TA修饰的Cu催化剂实现了63.6%的法拉第效率.
- 与原始Cu催化剂相比,TA修改显著提高了C2H4的选择性 (6.5倍以上).
- 现场研究和理论计算表明,TA的基稳定了Cuδ+和Cuδ+/Cu0接口,促进了CO二重化和C2H4的产生.
结论:
- 用酸进行现场分子工程有效控制Cu催化剂重建,用于选择性CO2到C2H4的转化.
- 该战略为从二氧化碳中增值化学品的生产提供了一条途径.
- 通过TA稳定Cuδ+和*COH中间体是促进C2H4选择性的关键.
关键词:
C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2H4C2C2H4C2C2C2C2C2C2C2C2C2C2C2C2C2C2C2这就是CO2RR的原因.Cuδ+/Cu0 的时间.气结合 气结合TA 分子 分子 分子
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