Interfacing Formate Dehydrogenase with Metal Oxides for the Reversible Electrocatalysis and Solar-Driven Reduction of Carbon Dioxide

Melanie Miller; William E. Robinson; Ana Rita Oliveira; Nina Heidary; Nikolay Kornienko; Julien Warnan; Inês A.C. Pereira; Erwin Reisner

doi:10.1002/anie.201814419

Interfacing Formate Dehydrogenase with Metal Oxides for the Reversible Electrocatalysis and Solar-Driven Reduction of Carbon Dioxide

Melanie Miller, William E. Robinson, Ana Rita Oliveira, Nina Heidary, Nikolay Kornienko, Julien Warnan, Inês A.C. Pereira, Erwin Reisner

Research output: Contribution to journal › Article

28 Citations (Scopus)

Abstract

The integration of enzymes with synthetic materials allows efficient electrocatalysis and production of solar fuels. Here, we couple formate dehydrogenase (FDH) from Desulfovibrio vulgaris Hildenborough (DvH) to metal oxides for catalytic CO ₂ reduction and report an in-depth study of the resulting enzyme–material interface. Protein film voltammetry (PFV) demonstrates the stable binding of FDH on metal-oxide electrodes and reveals the reversible and selective reduction of CO ₂ to formate. Quartz crystal microbalance (QCM) and attenuated total reflection infrared (ATR-IR) spectroscopy confirm a high binding affinity for FDH to the TiO ₂ surface. Adsorption of FDH on dye-sensitized TiO ₂ allows for visible-light-driven CO ₂ reduction to formate in the absence of a soluble redox mediator with a turnover frequency (TOF) of 11±1 s ⁻¹ . The strong coupling of the enzyme to the semiconductor gives rise to a new benchmark in the selective photoreduction of aqueous CO ₂ to formate.

Original language	English
Pages (from-to)	4601-4605
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	58
Issue number	14
DOIs	https://doi.org/10.1002/anie.201814419
Publication status	Published - 26 Mar 2019

Keywords

artificial photosynthesis
carbon dioxide fixation
formate dehydrogenase
interfaces
photocatalysis

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10.1002/anie.201814419

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Miller_et_al-2019-Angewandte_Chemie
Accepted author manuscript, 1.34 MB
Licence: CC BY-NC
Embargo ends: 22/01/21

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Miller, Melanie ; Robinson, William E. ; Oliveira, Ana Rita ; Heidary, Nina ; Kornienko, Nikolay ; Warnan, Julien ; Pereira, Inês A.C. ; Reisner, Erwin. / Interfacing Formate Dehydrogenase with Metal Oxides for the Reversible Electrocatalysis and Solar-Driven Reduction of Carbon Dioxide. In: Angewandte Chemie - International Edition. 2019 ; Vol. 58, No. 14. pp. 4601-4605.

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abstract = " The integration of enzymes with synthetic materials allows efficient electrocatalysis and production of solar fuels. Here, we couple formate dehydrogenase (FDH) from Desulfovibrio vulgaris Hildenborough (DvH) to metal oxides for catalytic CO 2 reduction and report an in-depth study of the resulting enzyme–material interface. Protein film voltammetry (PFV) demonstrates the stable binding of FDH on metal-oxide electrodes and reveals the reversible and selective reduction of CO 2 to formate. Quartz crystal microbalance (QCM) and attenuated total reflection infrared (ATR-IR) spectroscopy confirm a high binding affinity for FDH to the TiO 2 surface. Adsorption of FDH on dye-sensitized TiO 2 allows for visible-light-driven CO 2 reduction to formate in the absence of a soluble redox mediator with a turnover frequency (TOF) of 11±1 s −1 . The strong coupling of the enzyme to the semiconductor gives rise to a new benchmark in the selective photoreduction of aqueous CO 2 to formate. ",

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Interfacing Formate Dehydrogenase with Metal Oxides for the Reversible Electrocatalysis and Solar-Driven Reduction of Carbon Dioxide. / Miller, Melanie; Robinson, William E.; Oliveira, Ana Rita; Heidary, Nina; Kornienko, Nikolay; Warnan, Julien; Pereira, Inês A.C.; Reisner, Erwin.

In: Angewandte Chemie - International Edition, Vol. 58, No. 14, 26.03.2019, p. 4601-4605.

Research output: Contribution to journal › Article

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