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 (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).
Highlights
Efficient and noble metal-free water photolysis using sunlight is a primary focus of research to advance sustainable solar energy generation.[1]
Hydrogenases (H2ases) are H2-cycling enzymes and are by far the most efficient noble-metal-free electrocatalysts for H2 generation with an unrivalled turnover frequency (TOF) benchmark of more than 103 sÀ1 even at a modest overpotential.[3]. This excellent electrocatalytic activity of H2ases 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 H2ase is immobilized on Ru dye-sensitized TiO2 nanoparticles,[5] and on Cdcontaining quantum dots,[6] displaying excellent photocatalytic activity in sacrificial schemes
Photocatalytic H2 generation with such Ni bis(diphosphine) catalysts has only been achieved in combination with a costly Ru dye in purely aqueous solution.[9]
Summary
Efficient and noble metal-free water photolysis using sunlight is a primary focus of research to advance sustainable solar energy generation.[1]. Verçffentlicht von Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim www.angewandte.de 11723
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