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在功能化AU电极上电化学降低CO2

Yuxin Fang¹, John C Flake¹

¹Gordon and Mary Cain Department of Chemical Engineering, Louisiana State University , Baton Rouge, Louisiana 70803, United States.

Journal of the American Chemical Society

|February 10, 2017

概括

功能化的黄金电极可以通过电化学方法将二氧化碳 (CO2) 转化为有价值的燃料. 这种选择极大地改变了产品的选择性,为可再生能源储存提供了新的途径.

科学领域:

电化学
材料科学
储存可再生能源

背景情况:

电化学减少二氧化碳 (CO2) 是一种储存可再生能源在高密度燃料中的有希望的方法.
控制减少二氧化碳的产品选择性对于有效的能源转换至关重要.
功能化的电极提供了精确控制二氧化碳减排途径的潜力.

研究的目的:

为了研究醇结合联体对黄金 (Au) 表面二氧化碳的电化学减少的影响.
确定不同功能化的配体如何影响产品的选择性和效率.
探索潜在的调控选择性变化的机制.

主要方法:

在用三种不同的烯酸结合联体 (thiol-tethered ligands) 修改的金电极上进行了二氧化碳的电化学降解:二-烯酸,四-氨酸和氨酸.
分析了每一个修改过的电极的法拉达效率和产品分布 (形式,CO,H2).
为了解释观察到的选择性变化,提出了与体pKa相关的质子诱导脱吸机制.

主要成果:

与未经修改的黄金相比,用4-pyridinylethanemercaptan修改的黄金电极显示出法拉第效率增加了2倍,酸盐生产增加了3倍.
使用2 - 默卡普罗酸功能化的电极在演化反应中表现出近100%的法拉第效率.
修改后的电极导致一氧化碳 (CO) 和 (H2) 产量增加了两倍.

结论:

黄金表面的醇连接接物显著改变了电化学二氧化碳减排的选择性.
选择配体对于将二氧化碳减排指向特定产品,如甲酸盐,二氧化碳或气至关重要.
连接物 pKa 和相关的质子诱导脱吸机制是控制产品选择性的关键因素.

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