对于高度选择性二氧化碳电还原的阴离子溶解结构的分子工程
Wenpeng Ni1, Yongji Guan2, Houjun Chen1
1College of Materials Science and Engineering, Hunan University, Changsha, 410004, China.
Angewandte Chemie (International ed. in English)
|July 28, 2023
概括
分子工程调节水激活,用于选择性二氧化碳电还原 (CO2 RR). 接近的有机分子抑制进化 (HER) 并提高CO2RR选择性到99.2%的Ag薄膜.
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:
- 选择性二氧化碳电还原 (CO2 RR) 对可持续化学至关重要.
- 平衡水激活是提高二氧化碳RR对进化 (HER) 选择性的关键.
研究的目的:
- 开发一种分子工程策略,用于调节CO2 RR中的水激活.
- 通过控制接口水密度和质子供应物含量来提高二氧化碳RR选择性.
主要方法:
- 利用具有高古特曼捐赠人数的近极性有机小分子作为溶解调节器.
- 研究有机分子对K+溶解和电双层的影响.
- 使用二甲基硫氧化物 (DMSO) 作为KCl电解质 (KCl-DMSO-5) 的添加剂.
主要成果:
- 有机分子降低了界面水密度,抑制了HER.
- 吸附水中的弱化O-H键促进了解离,增强了CO2质子运动.
- 在Ag薄膜上达到99.2%的CO选择性和90.0%的Faradaic效率 (FECO) 在0.75~1.15V和RHE之间.
结论:
- 分子工程策略有效地调节了水激活的选择性CO2 RR.
- 这种方法可以扩展到其他金属电极 (Zn,Sn) 和有机分子 (例如N,N-二甲基形式胺).
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