Visible-light-driven CO<sub>2</sub>reduction to formate with a system of water-soluble zinc porphyrin and formate dehydrogenase in ionic liquid/aqueous media

Secundo, Francesco; Amao, Yutaka

doi:10.1039/d0ra08594d

Cited by 6 publications

(3 citation statements)

References 56 publications

(58 reference statements)

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“…Interestingly, this catalytic system retains its activity even in ionic liquid media. 217 Two viologen derivatives with carbamoyl groups (CV and CMV, Fig. 46c) were also synthesized and applied as electron carriers to the FDA-based photoinduced CO 2 -formic acid conversion system.…”

Section: Porphyrins For Co2 Reductionmentioning

confidence: 99%

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction

et al. 2022

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Section: Porphyrins For Co2 Reductionmentioning

confidence: 99%

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction

et al. 2022

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“…By maintaining the positive charge of a -CD-NHMe 2 + , a higher fraction of FDH molecules might orient via the distal FeS cluster, leading to the high activities for FDH photocatalysis reported in this work (Table S3). ,,,,− …”

Section: Resultsmentioning

confidence: 99%

Engineering Electro- and Photocatalytic Carbon Materials for CO₂ Reduction by Formate Dehydrogenase

et al. 2022

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Semiartificial approaches to renewable fuel synthesis exploit the integration of enzymes with synthetic materials for kinetically efficient fuel production. Here, a CO 2 reductase, formate dehydrogenase (FDH) from Desulfovibrio vulgaris Hildenborough, is interfaced with carbon nanotubes (CNTs) and amorphous carbon dots ( a -CDs). Each carbon substrate, tailored for electro- and photocatalysis, is functionalized with positive (−NHMe 2 + ) and negative (−COO – ) chemical surface groups to understand and optimize the electrostatic effect of protein association and orientation on CO 2 reduction. Immobilization of FDH on positively charged CNT electrodes results in efficient and reversible electrochemical CO 2 reduction via direct electron transfer with >90% Faradaic efficiency and −250 μA cm –2 at −0.6 V vs SHE (pH 6.7 and 25 °C) for formate production. In contrast, negatively charged CNTs only result in marginal currents with immobilized FDH. Quartz crystal microbalance analysis and attenuated total reflection infrared spectroscopy confirm the high binding affinity of active FDH to CNTs. FDH has subsequently been coupled to a -CDs, where the benefits of the positive charge (−NHMe 2 + -terminated a -CDs) were translated to a functional CD-FDH hybrid photocatalyst. High rates of photocatalytic CO 2 reduction (turnover frequency: 3.5 × 10 3 h –1 ; AM 1.5G) with dl -dithiothreitol as the sacrificial electron donor were obtained after 6 h, providing benchmark rates for homogeneous photocatalytic CO 2 reduction with metal-free light absorbers. This work provides a rational basis to understand interfacial surface/enzyme interactions at electrodes and photosensitizers to guide improvements with catalytic biohybrid materials.

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“…The TiO 2 j FDH photocatalyst oxidizes sugars or enzyme pre-treated cellulose to HCOO À while reducing CO 2 -to-HCOO À (Figure 1b). This system manages to perform CO 2 -to-HCOO À conversion without the requirement of costly NADH, [28][29][30] where electrons are provided through oxidation of waste substrates (e.g. cellulose) and channeled to FDH through TiO 2 acting as a light absorbing semiconductor.…”

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Comproportionation of CO₂ and Cellulose to Formate Using a Floating Semiconductor‐Enzyme Photoreforming Catalyst

et al. 2023

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Formate production via both CO2 reduction and cellulose oxidation in a solar‐driven process is achieved by a semi‐artificial biohybrid photocatalyst consisting of immobilized formate dehydrogenase on titanium dioxide (TiO2|FDH) producing up to 1.16±0.04 mmolformate g TiO2 ${{_{\ {\rm TiO}{_{2}}}}}$ −1 in 24 hours at 30 °C and 101 kPa under anaerobic conditions. Isotopic labeling experiments with 13C‐labeled substrates support the mechanism of stoichiometric formate formation through both redox half‐reactions. TiO2|FDH was further immobilized on hollow glass microspheres to perform more practical floating photoreforming allowing vertical solar light illumination with optimal light exposure of the photocatalyst to real sunlight. Enzymatic cellulose depolymerization coupled to the floating photoreforming catalyst generates 0.36±0.04 mmolformate per m2 irradiation area after 24 hours. This work demonstrates the synergistic solar‐driven valorization of solid and gaseous waste streams using a biohybrid photoreforming catalyst in aqueous solution and will thus provide inspiration for the development of future semi‐artificial waste‐to‐chemical conversion strategies.

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Visible-light-driven CO₂reduction to formate with a system of water-soluble zinc porphyrin and formate dehydrogenase in ionic liquid/aqueous media

Abstract: Visible-light-driven CO2 reduction to formate with water-soluble zinc tetraphenylporphyrin tetrasulfonate, formate dehydrogenase from Candida boidinii and methylviologen in the presence of triethanolamine as an electron donor in an ionic liquid.

Cited by 6 publications

References 56 publications

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction

Engineering Electro- and Photocatalytic Carbon Materials for CO₂ Reduction by Formate Dehydrogenase

Comproportionation of CO₂ and Cellulose to Formate Using a Floating Semiconductor‐Enzyme Photoreforming Catalyst

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Visible-light-driven CO2reduction to formate with a system of water-soluble zinc porphyrin and formate dehydrogenase in ionic liquid/aqueous media

Abstract: Visible-light-driven CO2 reduction to formate with water-soluble zinc tetraphenylporphyrin tetrasulfonate, formate dehydrogenase from Candida boidinii and methylviologen in the presence of triethanolamine as an electron donor in an ionic liquid.

Cited by 6 publications

References 56 publications

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H2production and CO2reduction

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H2production and CO2reduction

Engineering Electro- and Photocatalytic Carbon Materials for CO2 Reduction by Formate Dehydrogenase

Comproportionation of CO2 and Cellulose to Formate Using a Floating Semiconductor‐Enzyme Photoreforming Catalyst

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Visible-light-driven CO₂reduction to formate with a system of water-soluble zinc porphyrin and formate dehydrogenase in ionic liquid/aqueous media

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction

Engineering Electro- and Photocatalytic Carbon Materials for CO₂ Reduction by Formate Dehydrogenase

Comproportionation of CO₂ and Cellulose to Formate Using a Floating Semiconductor‐Enzyme Photoreforming Catalyst