Ultimate downsizing of d-fructose dehydrogenase for improving the performance of direct electron transfer-type bioelectrocatalysis

Kaida, Yuya; Hibino, Yuya; Kitazumi, Yuki; Shirai, Osamu; Kano, Kenji

doi:10.1016/j.elecom.2018.12.001

Cited by 37 publications

(34 citation statements)

References 25 publications

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“…On the other hand, a Δ1c2c_FDH variant, which lacked both the heme 1c and 2c moieties, showed a DET-type bioelectrocatalytic wave that was very similar to that of M450QΔ1c_FDH [60]: an increase in the limiting catalytic current density caused by the downsizing of the enzyme and a decrease in the overpotential thanks to the direct heterogeneous electron transfer from heme 3c with the most negative formal potential to an electrode. The DET-type bioelectrocatalytic waves of these FDH variants are shown in Figure 10.…”

Section: Protein Engineering Methods For the Improvement Of Det-type mentioning

confidence: 94%

Direct Electron Transfer-Type Bioelectrocatalysis of Redox Enzymes at Nanostructured Electrodes

et al. 2020

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Direct electron transfer (DET)-type bioelectrocatalysis, which couples the electrode reactions and catalytic functions of redox enzymes without any redox mediator, is one of the most intriguing subjects that has been studied over the past few decades in the field of bioelectrochemistry. In order to realize the DET-type bioelectrocatalysis and improve the performance, nanostructures of the electrode surface have to be carefully tuned for each enzyme. In addition, enzymes can also be tuned by the protein engineering approach for the DET-type reaction. This review summarizes the recent progresses in this field of the research while considering the importance of nanostructure of electrodes as well as redox enzymes. This review also describes the basic concepts and theoretical aspects of DET-type bioelectrocatalysis, the significance of nanostructures as scaffolds for DET-type reactions, protein engineering approaches for DET-type reactions, and concepts and facts of bidirectional DET-type reactions from a cross-disciplinary viewpoint.

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Section: Protein Engineering Methods For the Improvement Of Det-type mentioning

confidence: 94%

Direct Electron Transfer-Type Bioelectrocatalysis of Redox Enzymes at Nanostructured Electrodes

et al. 2020

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“…S2(B)) in order to increase the surface concentrations due to the ¦1c2c-downsizing and realize a short-cut electron transfer from heme 3c to electrodes directly. 31 According to the above two expectations, the variant may lead to an increase in the limiting current density and the decrease in the overpotential, respectively, in the DET-type bioelectrocatalytic oxidation of D-fructose. The expected short-cut electron transfer from heme 3c to a planar Au electrode seems to be realized, 31 though further study will be required to verify the proposed electron transfer pathway.…”

Section: Introductionmentioning

confidence: 98%

“…31 According to the above two expectations, the variant may lead to an increase in the limiting current density and the decrease in the overpotential, respectively, in the DET-type bioelectrocatalytic oxidation of D-fructose. The expected short-cut electron transfer from heme 3c to a planar Au electrode seems to be realized, 31 though further study will be required to verify the proposed electron transfer pathway. However, contrast to our expectation, its limiting catalytic current density was lower than that of ¦1cFDH.…”

Section: Introductionmentioning

confidence: 98%

Discussion on Direct Electron Transfer-Type Bioelectrocatalysis of Downsized and Axial-Ligand Exchanged Variants of d-Fructose Dehydrogenase

et al. 2020

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D-Fructose dehydrogenase (FDH) gives a clear direct electron transfer (DET)-type bioelectrocatalytic wave even at planar gold (Au) electrodes. The recombinant (native) FDH (r_FDH) has three hemes c in subunit II (1c, 2c, and 3c from N-terminus). With a view to downsize the enzyme and shorten the distance between an electrode-active site and an electrode, we constructed a variant that lacked 143 amino acid residues involving the heme 1c moiety (Δ1cFDH) and a variant that lacked 199 amino acid residues involving the heme 1c and 2c moieties (Δ1c2cFDH). In order to shift the redox potential of heme 2c of Δ1cFDH to the negative direction, the M450 residue as the axial 6th ligand of heme 2c was also replaced with glutamine (M450QΔ1cFDH). The DET-type catalytic properties of r_FDH and the three variants at planar Au electrodes were compared with each other, and the steady-state waves were analyzed on a random orientation model. The orientation of the enzymes on the electrode was also discussed. In addition, in order to examine the electron transfer pathway in the DETtype reaction of Δ1c2cFDH, ESR measurements and inhibition of DET-type reaction by cyanide ion were performed.

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“…On the other hand, a Δ1c2c_FDH variant, which lacks both the heme 1c and 2c moieties, showed DET-type bioelectrocatalytic activity similar to that of M450QΔ1c_FDH were realized [57]: an increase in the limiting catalytic current density caused by the downsizing of the enzyme and a decrease in the overpotential thanks to the heterogeneous electron transfer from heme 3c with the most negative formal potential to an electrode. DET-type bioelectrocatalytic waves of these FDH variants are shown in Figure 10.…”

Section: Nanoporous Metals and Aggregated Metal Nanoparticlesmentioning

confidence: 99%

Direct Electron Transfer-type Bioelectrocatalysis of Redox Enzymes at Nanostructured Electrodes

Adachi¹,

Kitazumi²,

Shirai³

et al. 2020

Preprint

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Direct electron transfer (DET)-type bioelectrocatalysis, which couples electrode reactions and catalytic functions of redox enzymes without any redox mediator, is one of the most intriguing subjects studied over the past decades in the field of bioelectrochemistry. In order to realize the DET-type bioelectrocatalysis and to improve the performance, nanostructures of the electrode surface have to be carefully tuned for each enzyme. In addition, enzymes can also be tuned by protein engineering approach for the DET-type reaction. This review summarizes the resent progresses in this field of the research, while taking into consideration of the importance of nanostructure of electrodes as well as redox enzymes. Described are basic concepts and theoretical aspects of DET-type bioelectrocatalysis, significance of nanostructures as scaffolds for DET-type reactions, protein engineering approached for DET-type reactions, and concepts and facts of bidirectional DET-type reactions, from a cross-disciplinary viewpoint.

show abstract

Ultimate downsizing of d-fructose dehydrogenase for improving the performance of direct electron transfer-type bioelectrocatalysis

Cited by 37 publications

References 25 publications

Direct Electron Transfer-Type Bioelectrocatalysis of Redox Enzymes at Nanostructured Electrodes

Direct Electron Transfer-Type Bioelectrocatalysis of Redox Enzymes at Nanostructured Electrodes

Discussion on Direct Electron Transfer-Type Bioelectrocatalysis of Downsized and Axial-Ligand Exchanged Variants of d-Fructose Dehydrogenase

Direct Electron Transfer-type Bioelectrocatalysis of Redox Enzymes at Nanostructured Electrodes

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