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用分子钴催化剂功能化的光电阴极用于水中二氧化碳的选择性还原。

Photocathode functionalized with a molecular cobalt catalyst for selective carbon dioxide reduction in water.

作者信息

Pati Palas Baran, Wang Ruwen, Boutin Etienne, Diring Stéphane, Jobic Stéphane, Barreau Nicolas, Odobel Fabrice, Robert Marc

机构信息

Université de Nantes, CNRS, CEISAM UMR 6230, F-44000, Nantes, France.

Université de Paris, Laboratoire d'Electrochimie Moléculaire, CNRS, F-75006, Paris, France.

出版信息

Nat Commun. 2020 Jul 13;11(1):3499. doi: 10.1038/s41467-020-17125-4.

Abstract

Artificial photosynthesis is a vibrant field of research aiming at converting abundant, low energy molecules such as water, nitrogen or carbon dioxide into fuels or useful chemicals by means of solar energy input. Photo-electrochemical reduction of carbon dioxide is an appealing strategy, aiming at reducing the greenhouse gas into valuable products such as carbon monoxide at low or without bias voltage. Yet, in such configuration, there is no catalytic system able to produce carbon monoxide selectively in aqueous media with high activity, and using earth-abundant molecular catalyst. Upon associating a p-type Cu(In,Ga)Se semi-conductor with cobalt quaterpyridine complex, we herein report a photocathode complying with the aforementioned requirements. Pure carbon dioxide dissolved in aqueous solution (pH 6.8) is converted to carbon monoxide under visible light illumination with partial current density above 3 mA cm and 97% selectivity, showing good stability over time.

摘要

人工光合作用是一个充满活力的研究领域,旨在通过输入太阳能将丰富的低能量分子(如水、氮或二氧化碳)转化为燃料或有用的化学品。二氧化碳的光电化学还原是一种有吸引力的策略,旨在在低偏压或无偏压的情况下将温室气体还原为有价值的产品,如一氧化碳。然而,在这种配置中,没有催化系统能够在水性介质中以高活性选择性地生产一氧化碳,并且使用地球上丰富的分子催化剂。通过将p型Cu(In,Ga)Se半导体与钴四吡啶配合物结合,我们在此报告了一种符合上述要求的光电阴极。溶解在水溶液(pH 6.8)中的纯二氧化碳在可见光照射下被转化为一氧化碳,其部分电流密度高于3 mA cm,选择性为97%,并且随着时间的推移显示出良好的稳定性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5212/7358214/a11edc2de10e/41467_2020_17125_Fig1_HTML.jpg

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