Efficient, Light-Driven Reduction of CO2 to CO by a Carbon Monoxide Dehydrogenase–CdSe/CdS Nanorod Photosystem

The solar conversion of CO2 to low carbon fuels has been heralded as a potential solution to combat the rise in greenhouse gas emissions. Here we report the first light-driven activation of [NiFe] CODH II from Carboxydothermus hydrogenoformans for the reduction of CO2 to CO. To accomplish this, a hy...

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Veröffentlicht in:The journal of physical chemistry letters 2022-06, Vol.13 (24), p.5553-5556
Hauptverfasser: White, David W., Esckilsen, Daniel, Lee, Seung Kyu, Ragsdale, Stephen W., Dyer, R. Brian
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Sprache:eng
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Zusammenfassung:The solar conversion of CO2 to low carbon fuels has been heralded as a potential solution to combat the rise in greenhouse gas emissions. Here we report the first light-driven activation of [NiFe] CODH II from Carboxydothermus hydrogenoformans for the reduction of CO2 to CO. To accomplish this, a hybrid photosystem composed of CODH II and CdSe/CdS dot-in-rod nanocrystals was developed. By incorporating a low-potential redox mediator to assist electron transfer, quantum yields up to 19% and turnover frequencies of 9 s–1 were achieved. These results represent a new standard in efficient CO2 reduction by an enzyme-based photocatalytic systems. Furthermore, successful photoactivation of CODH II allows for future exploration into the enzyme’s not fully understood mechanism.
ISSN:1948-7185
1948-7185
DOI:10.1021/acs.jpclett.2c01412