Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning |
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| Authors: | Dr Michael G Allan Thomas Pichon Dr Jade A McCune Dr Christine Cavazza Dr Alan Le Goff Dr Moritz F Kühnel |
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| Institution: | 1. Department of Chemistry, Faculty of Science and Engineering, Swansea University, Singleton Park, Swansea, SA2 8PP Wales, UK;2. Univ. Grenoble Alpes, CEA, CNRS, IRIG, CBM, 38000 Grenoble, France;3. Melville Laboratory for Polymer Synthesis, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW UK;4. University Grenoble Alpes, CNRS, DCM UMR 5250, F-38000 Grenoble, France |
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| Abstract: | This work showcases the performance of NiFeSe] hydrogenase from Desulfomicrobium baculatum for solar-driven hydrogen generation in a variety of organic-based deep eutectic solvents. Despite its well-known sensitivity towards air and organic solvents, the hydrogenase shows remarkable performance under an aerobic atmosphere in these solvents when paired with a TiO2 photocatalyst. Tuning the water content further increases hydrogen evolution activity to a TOF of 60±3 s−1 and quantum yield to 2.3±0.4 % under aerobic conditions, compared to a TOF of 4 s−1 in a purely aqueous solvent. Contrary to common belief, this work therefore demonstrates that placing natural hydrogenases into non-natural environments can enhance their intrinsic activity beyond their natural performance, paving the way for full water splitting using hydrogenases. |
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| Keywords: | Deep Eutectic Solvents Hydrogen Hydrogenase Oxygen Tolerance Photocatalysis |
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