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. 2014 Oct 20;53(43):11538-42.
doi: 10.1002/anie.201406811. Epub 2014 Sep 9.

Photocatalytic hydrogen production using polymeric carbon nitride with a hydrogenase and a bioinspired synthetic Ni catalyst

Christine A Caputo  1 , Manuela A Gross, Vincent W Lau, Christine Cavazza, Bettina V Lotsch, Erwin Reisner
Affiliations

Photocatalytic hydrogen production using polymeric carbon nitride with a hydrogenase and a bioinspired synthetic Ni catalyst

Christine A Caputo et al. Angew Chem Int Ed Engl. .

Abstract

Solar-light-driven H2 production in water with a [NiFeSe]-hydrogenase (H2ase) and a bioinspired synthetic nickel catalyst (NiP) in combination with a heptazine carbon nitride polymer, melon (CN(x)), is reported. The semibiological and purely synthetic systems show catalytic activity during solar light irradiation with turnover numbers (TONs) of more than 50,000 mol H2(mol H2ase)(-1) and approximately 155 mol H2 (mol NiP)(-1) in redox-mediator-free aqueous solution at pH 6 and 4.5, respectively. Both systems maintained a reduced photoactivity under UV-free solar light irradiation (λ>420 nm).

Keywords: carbon nitride; enzyme catalysis; hydrogen production; hydrogenases; photocatalysis.

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Figures

Figure 1
Figure 1
Representation of the photo-H2 production with CNx and Dmb [NiFeSe]-H2ase (PDB ID: 1CC1)[15a] or CNx and NiP (counterions omitted) in aqueous EDTA solution. Irradiation of CNx results in the photoinduced direct electron transfer to the catalysts with H2 formation and hole quenching in CNx by EDTA.
Figure 2
Figure 2
H2 production under optimized conditions using Dmb [NiFeSe]-H2ase (50 pmol) in EDTA (pH 6, 0.1 m, 3 mL) and CNx (5 mg) under 1 sun irradiation in the absence (λ>300 nm) and presence of a 420 nm UV filter. Control experiments without EDTA, CNx, or H2ase are also shown.
Figure 3
Figure 3
H2 production under optimized conditions using NiP (20 nmol) in aqueous EDTA (0.1 m, pH 4.5, 3 mL) and CNx (5 mg) under 1 sun irradiation. Data collected under standard conditions (λ>300 nm), with UV-light-filtered irradiation (λ>420 nm) and control experiments without NiP catalyst or CNx are also shown.
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References

    1. pp. 3285–3288.
    1. Ott S, Kritikos M, Åkermark B, Sun L. Angew. Chem. Int. Ed. 42 - PubMed
    2. Angew. Chem. 2003;115
    1. Reece SY, Hamel JA, Sung K, Jarvi TD, Esswein AJ, Pijpers JJH, Nocera DG. Science. 2003;334 - PubMed
    1. McKone JR, Lewis NS, Gray HB. Chem. Mater. 2011;26
    1. Lin C-Y, Lai Y-H, Mersch D, Reisner E. Chem. Sci. 2014;3

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