Photoelectrochemical hybrid cell for unbiased CO2 reduction coupled to alcohol oxidation
Photoelectrochemical hybrid cell for unbiased CO2 reduction coupled to alcohol oxidation
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DOI：
10.1038/s44160-021-00003-2
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发表时间：
2022-01-01
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影响因子：
--
通讯作者：
Reisner, Erwin
中科院分区：
文献类型：
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作者：
Anton-Garcia, Daniel;Moore, Esther Edwardes;Reisner, Erwin
将二氧化碳还原为可再生燃料必须与可持续的氧化过程相结合，以设计出生产太阳能燃料的可行装置。在光电化学电池中，水氧化成O-2是主要的氧化反应，并且当与CO2还原结合时通常需要一对光吸收剂或施加的偏压。在这里，我们报告了一个无偏压的光电化学装置，同时CO2还原为甲酸和醇氧化为醛在水溶液中的条件。该光阳极通过将基于二酮基吡咯并吡咯的发色团和基于硝酰基的醇氧化催化剂共固定在介孔TiO 2支架上而构建，其提供了无贵金属的染料敏化光阳极。光电阳极连接到生物混合阴极，该生物混合阴极由整合到介孔氧化铟锡电极中的CO2还原酶甲酸脱氢酶组成。无偏压电池在可见光照射下可提供高达30 μ A cm（-2）的持续光电流，从而同时产生醛和甲酸。我们的研究结果表明，在没有外部偏压的情况下，单光吸收体光电化学电池可用于并行燃料生产和化学合成从CO2和醇类底物。
The reduction of CO2 to renewable fuels must be coupled to a sustainable oxidation process to devise a viable device that produces solar fuels. In photoelectrochemical cells, water oxidation to O-2 is the predominant oxidation reaction and typically requires a pair of light absorbers or an applied bias voltage when coupled to CO2 reduction. Here, we report a bias-free photoelectrochemical device for simultaneous CO2 reduction to formate and alcohol oxidation to aldehyde in aqueous conditions. The photoanode is constructed by co-immobilization of a diketopyrrolopyrrole-based chromophore and a nitroxyl-based alcohol oxidation catalyst on a mesoporous TiO2 scaffold, which provides a precious-metal-free dye-sensitized photoanode. The photoanode is wired to a biohybrid cathode that consists of the CO2 reduction enzyme formate dehydrogenase integrated into a mesoporous indium tin oxide electrode. The bias-free cell delivers sustained photocurrents of up to 30 mu A cm(-2) under visible-light irradiation, which results in simultaneous aldehyde and formate production. Our results show that in the absence of an external bias, single light absorber photoelectrochemical cells can be used for parallel fuel production and chemical synthesis from CO2 and alcohol substrates.