Abstract
Solar-driven coupling of water oxidation with CO2 reduction sustains life on our planet and is of high priority in contemporary energy research. Here, we report a photoelectrochemical tandem device that performs photocatalytic reduction of CO2 to formate. We employ a semi-artificial design, which wires a W-dependent formate dehydrogenase (FDH) cathode to a photoanode containing the photosynthetic water oxidation enzyme, Photosystem II, via a synthetic dye with complementary light absorption. From a biological perspective, the system achieves a metabolically inaccessible pathway of light-driven CO2 fixation to formate. From a synthetic point of view, it represents a proof-of-principle system utilizing precious-metal-free catalysts for selective CO2-to-formate conversion using water as an electron donor. This hybrid platform demonstrates the translatability and versatility of coupling abiotic and biotic components to create challenging models for solar fuel and chemical synthesis.
Highlights
I n the thylakoid membrane of plants, light-driven water oxidation in the photosynthetic Z-scheme is coupled to CO2 fixation for sugar synthesis via the dark Calvin−Benson− Bassham (CBB) cycle.[1,2]
The CBB cycle involves significant adenosine triphosphate (ATP) consumption, which leads to a lower biomass production efficiency compared to the prokaryotic reductive acetyl-coenzyme A pathway.[6]
Artificial photosynthesis aspires to couple solar-light-driven water oxidation with CO2 reduction to chemical fuels at higher efficiency than natural systems.[16]
Summary
I n the thylakoid membrane of plants, light-driven water oxidation in the photosynthetic Z-scheme is coupled to CO2 fixation for sugar synthesis via the dark Calvin−Benson− Bassham (CBB) cycle (eq 1).[1,2] this solar-energy-. We employ a semi-artificial design, which wires a Wdependent formate dehydrogenase (FDH) cathode to a photoanode containing the photosynthetic water oxidation enzyme, Photosystem II, via a synthetic dye with complementary light absorption.
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