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Efficient, Light-Driven Reduction of CO<sub>2</sub> to CO by a Carbon Monoxide Dehydrogenase–CdSe/CdS Nanorod Photosystem

David W. White, Daniel Esckilsen, Seung Kyu Lee, Stephen W. Ragsdale, R. Brian Dyer

2022The Journal of Physical Chemistry Letters10 citationsDOIOpen Access PDF

Abstract

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.

Topics & Concepts

NanorodCarbon monoxide dehydrogenaseCarbon monoxidePhotosystem IIPhotochemistryReduction (mathematics)Artificial photosynthesisChemistryPhotosystem IPhotosynthesisMaterials scienceNanotechnologyPhotocatalysisCatalysisBiochemistryGeometryMathematicsCO2 Reduction Techniques and CatalystsAdvanced Photocatalysis TechniquesMicrobial Fuel Cells and Bioremediation
Efficient, Light-Driven Reduction of CO<sub>2</sub> to CO by a Carbon Monoxide Dehydrogenase–CdSe/CdS Nanorod Photosystem | Litcius