Photoelectrochemical CO2 Reduction with a Rhenium Organometallic Redox Mediator at Semiconductor/Aqueous Liquid Junction Interfaces

Electrochemical and photoelectrochemical CO2 reductions were carried out with Re(bh‐bipy)(CO)3(OH2) cocatalysts in aqueous electrolytes. Competition between hydrogen evolution and CO2 reduction was observed under (photo)electrochemical conditions for both glassy carbon and CuInS2 electrodes. The par...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2019-11, Vol.58 (46), p.16395-16399
Main Authors: Chae, Sang Youn, Choi, Ja Youn, Kim, Yoolim, Le Tri Nguyen, Dang, Joo, Oh‐Shim
Format: Article
Language:English
Subjects:
Aqueous electrolytes
Carbon dioxide
Carbon monoxide
Chemical reduction
Current density
Electrochemistry
Electrodes
Electrolysis
Glassy carbon
Hydrogen evolution
Interfaces
Rhenium
Selectivity
solar energy
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Summary:Electrochemical and photoelectrochemical CO2 reductions were carried out with Re(bh‐bipy)(CO)3(OH2) cocatalysts in aqueous electrolytes. Competition between hydrogen evolution and CO2 reduction was observed under (photo)electrochemical conditions for both glassy carbon and CuInS2 electrodes. The partial current density for CO generation is limited even though the additional potential is applied. However, electrochemical hydrogen evolution was suppressed under photoelectrochemical conditions, and the selectivity and partial current density for CO were considerably increased when compared to the electrochemical reduction in an identical electrode/electrolyte system. This finding may provide insights into using semiconductor/liquid junctions for solar fuel devices to overcome the limitations of electrolysis systems with an external bias. On the surface: The selectivity for either hydrogen evolution or CO2 reduction can be controlled by using either electrical energy or photon energy. Competition between hydrogen evolution and CO2 reduction was observed under electrochemical conditions for both glassy carbon and CuInS2 electrodes. However, electrochemical hydrogen evolution was suppressed under photoelectrochemical conditions, showing selectivity for CO2 reduction using an identical electrode/electrolyte system.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201908398