Photoelectrochemical Reduction of Carbon Dioxide with a Copper Graphitic Carbon Nitride Photocathode,Chemistry - A European Journal

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Photoelectrochemical Reduction of Carbon Dioxide with a Copper Graphitic Carbon Nitride Photocathode
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2021-07-18 , DOI: 10.1002/chem.202101820
Huijun Yu ₁ , Hagai Cohen ₂ , Ronny Neumann ₁

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Research on the photoreduction of CO₂ often has been dominated by the use of sacrificial reducing agents. A pathway that avoids this problem would be the development of photocathodes for CO₂ reduction that could then be coupled to a photoanodic oxygen evolution reaction. Here, we present the use of copper-substituted graphitic carbon nitride (Cu−CN) on a fluorinated tin oxide (FTO) electrode for the photoelectrochemical two-electron reduction of CO₂ to CO as a major product (>95 %) and formic acid (<5 %). The results show that at a potential of −2.5 V versus Fc\Fc⁺ the CO₂ reduction activity of Cu−CN on FTO electrode improves by 25 % upon illumination by visible light with a faradaic efficiency of nearly 100 %. Independently, X-ray photoelectron spectroscopy conclusively shows a pronounced increase in the electrical conductivity of the Cu−CN upon white light illumination under vacuum and a contactless measuring configuration. This photo-assisted charge mobility is shown to play a key role in the increased reactivity and faradaic efficiency for the reduction of CO₂.

中文翻译：

用铜石墨碳氮化物光电阴极光电化学还原二氧化碳

CO ₂光还原的研究通常以牺牲还原剂的使用为主。避免这个问题的途径是开发用于 CO ₂还原的光阴极，然后可以将其与光阳极析氧反应耦合。在这里，我们介绍了在氟化氧化锡 (FTO) 电极上使用铜取代的石墨碳氮化物 (Cu-CN) 将 CO ₂光电化学双电子还原为 CO 作为主要产物 (> 95 %) 和甲酸酸 (<5%)。结果表明，在 -2.5 V 的电位下，Fc\Fc ⁺ CO ₂在可见光照射下，FTO 电极上 Cu-CN 的还原活性提高了 25%，法拉第效率接近 100%。独立地，X 射线光电子能谱最终显示在真空和非接触式测量配置下，在白光照射下 Cu-CN 的电导率显着增加。显示这种光辅助电荷迁移率在增加还原 CO _{2 的}反应性和法拉第效率方面起着关键作用。

更新日期：2021-09-24

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