Photocatalytic Hydrogen Evolution with a Hydrogenase in a Mediator‐Free System under High Levels of Oxygen

Sakai, Tsubasa; Mersch, Dirk; Reisner, Erwin

doi:10.1002/anie.201306214

Cited by 133 publications

(112 citation statements)

References 53 publications

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“…34,35 Thus, [NiFeSe]-H 2 ase allows for the efficient formation and accumulation of H 2 during the water-splitting process, where O 2 is also generated as a byproduct. 36 [NiFeSe]-H 2 ase was drop-cast onto the IO-mesoITO electrode, and excess H 2 ase removed by rinsing with the electrolyte solution before being used in electrochemical studies. The electrocatalytic response of D. baculatum [NiFeSe]-H 2 ase on the IO-mesoITO electrode under different conditions is summarized in Figure 3 and Supporting Information Figure S7.…”

Section: Journal Of the American Chemical Societymentioning

confidence: 99%

Wiring of Photosystem II to Hydrogenase for Photoelectrochemical Water Splitting

et al. 2015

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In natural photosynthesis, light is used for the production of chemical energy carriers to fuel biological activity. The re-engineering of natural photosynthetic pathways can provide inspiration for sustainable fuel production and insights for understanding the process itself. Here, we employ a semiartificial approach to study photobiological water splitting via a pathway unavailable to nature: the direct coupling of the water oxidation enzyme, photosystem II, to the H2 evolving enzyme, hydrogenase. Essential to this approach is the integration of the isolated enzymes into the artificial circuit of a photoelectrochemical cell. We therefore developed a tailor-made hierarchically structured indium-tin oxide electrode that gives rise to the excellent integration of both photosystem II and hydrogenase for performing the anodic and cathodic half-reactions, respectively. When connected together with the aid of an applied bias, the semiartificial cell demonstrated quantitative electron flow from photosystem II to the hydrogenase with the production of H2 and O2 being in the expected two-to-one ratio and a light-to-hydrogen conversion efficiency of 5.4% under low-intensity red-light irradiation. We thereby demonstrate efficient light-driven water splitting using a pathway inaccessible to biology and report on a widely applicable in vitro platform for the controlled coupling of enzymatic redox processes to meaningfully study photocatalytic reactions.

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Section: Journal Of the American Chemical Societymentioning

confidence: 99%

Wiring of Photosystem II to Hydrogenase for Photoelectrochemical Water Splitting

et al. 2015

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“…Reisner and co-workers used Eosin Y, a polyaromatic photosensitiser that drives H 2 evolution by [NiFeSe]-H2ase through efficient bimolecular ET, without the need for a redox mediator, using triethanolamine (TEOA) as sacrificial donor [44]. The powerfully reducing nature of excited Eosin (E = À0.91 V vs. NHE) also ensured adequate O 2 tolerance.…”

Section: Configurationsmentioning

confidence: 99%

Solar-driven proton and carbon dioxide reduction to fuels — lessons from metalloenzymes

Bachmeier

Armstrong

2015

Current Opinion in Chemical Biology

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“…[3] This excellent electrocatalytic activity of H 2 ases was exploited in photocatalytic schemes with a light absorber in the absence of a soluble redox mediator: a homogeneous photocatalytic system with a molecular organic dye,[4] and semiheterogeneous systems, in which the H 2 ase is immobilized on Ru dye-sensitized TiO 2 nanoparticles,[5] and on Cd-containing quantum dots,[6] displaying excellent photocatalytic activity in sacrificial schemes.…”

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“…We selected Desulfomicrobium baculatum ( Dmb ) [NiFeSe]-H 2 ase because of its well-known[15] and excellent H 2 evolution rate as well as tolerance toward H 2 and O 2 , allowing for the accumulation of H 2 during irradiation and the handling of the enzyme in the absence of strictly anaerobic conditions. [4], [5], [15b]…”

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Photocatalytic Hydrogen Production using Polymeric Carbon Nitride with a Hydrogenase and a Bioinspired Synthetic Ni Catalyst

et al. 2014

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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 (CNx), 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).

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Photocatalytic Hydrogen Evolution with a Hydrogenase in a Mediator‐Free System under High Levels of Oxygen

Abstract: Take a breath: An oxygen‐tolerant hydrogenase can be employed with a dye in a photocatalytic scheme for the generation of H2. The homogeneous system does not require a redox mediator and visible‐light irradiation yields high amounts of H2 even in the presence of air.

Cited by 133 publications

References 53 publications

Wiring of Photosystem II to Hydrogenase for Photoelectrochemical Water Splitting

Wiring of Photosystem II to Hydrogenase for Photoelectrochemical Water Splitting

Solar-driven proton and carbon dioxide reduction to fuels — lessons from metalloenzymes

Photocatalytic Hydrogen Production using Polymeric Carbon Nitride with a Hydrogenase and a Bioinspired Synthetic Ni Catalyst

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