Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning

Allan, Michael; Pichon, Thomas; McCune, Jade A.; Cavazza, Christine; Goff, Alan Le; Kuehnel, Moritz

doi:10.1002/anie.202219176

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Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning

Michael Allan, Thomas Pichon, Jade A. McCune

, Christine Cavazza, Alan Le Goff

, Moritz Kuehnel

Angewandte Chemie International Edition, Volume: 62, Issue: 22

Swansea University Authors: Michael Allan, Moritz Kuehnel

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DOI (Published version): 10.1002/anie.202219176

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 und...

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Published in:	Angewandte Chemie International Edition
ISSN:	1433-7851 1521-3773
Published:	Wiley 2023
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URI:	https://cronfa.swan.ac.uk/Record/cronfa63074
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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.</abstract><type>Journal Article</type><journal>Angewandte Chemie International Edition</journal><volume>62</volume><journalNumber>22</journalNumber><paginationStart/><paginationEnd/><publisher>Wiley</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>1433-7851</issnPrint><issnElectronic>1521-3773</issnElectronic><keywords>Deep Eutectic Solvents, Hydrogen, Hydrogenase,Oxygen Tolerance, Photocatalysis</keywords><publishedDay>22</publishedDay><publishedMonth>5</publishedMonth><publishedYear>2023</publishedYear><publishedDate>2023-05-22</publishedDate><doi>10.1002/anie.202219176</doi><url>http://dx.doi.org/10.1002/anie.202219176</url><notes/><college>COLLEGE NANME</college><department>Chemistry</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>CHEM</DepartmentCode><institution>Swansea University</institution><apcterm>SU Library paid the OA fee (TA Institutional Deal)</apcterm><funders>Swansea University. 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spelling	v2 63074 2023-04-04 Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning b1f40243f0e1ee0ec5aa706601527f6a Michael Allan Michael Allan true false 210dbad181ce095d6f8bf2bd1d616d4e 0000-0001-8678-3779 Moritz Kuehnel Moritz Kuehnel true false 2023-04-04 CHEM 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. Journal Article Angewandte Chemie International Edition 62 22 Wiley 1433-7851 1521-3773 Deep Eutectic Solvents, Hydrogen, Hydrogenase,Oxygen Tolerance, Photocatalysis 22 5 2023 2023-05-22 10.1002/anie.202219176 http://dx.doi.org/10.1002/anie.202219176 COLLEGE NANME Chemistry COLLEGE CODE CHEM Swansea University SU Library paid the OA fee (TA Institutional Deal) Swansea University. This work was supported by EPSRC through a DTA studentship to M.G.A. (EP/R51312X/1), and a capital investment grant to M.F.K. (EP/S017925/1), by Universities Wales through the Global Wales International Research Mobility Fund (UNIW/RMF-SU/07) and by HEFCW through the Research Wales Innovation Fund Collaboration Booster. We thank Swansea University for providing start-up funds to M.F.K. and support through the Swansea-Grenoble Collaboration Fund. This work was supported by the Agence Nationale de la Recherche through the LabEx ARCANE program (ANR-11-LABX-0003-01), the Graduate School on Chemistry, Biology and Health of Univ. Grenoble Alpes CBH-EUR-GS (ANR-17-EURE-0003) and by the CFR PhD program-CEA (PhD funding for T.P.). We thank Dr. Oliver Lenz and Dr. Stefan Frielingsdorf (TU Berlin) and Prof. Frank Marken (Bath) for helpful discussions. 2023-07-06T16:08:41.6881951 2023-04-04T09:16:08.9982880 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Michael Allan 1 Thomas Pichon 2 Jade A. McCune 0000-0001-5048-2683 3 Christine Cavazza 4 Alan Le Goff 0000-0002-6765-5859 5 Moritz Kuehnel 0000-0001-8678-3779 6 63074__28050__3173a2e64a804683ac541952d7c2acb4.pdf 63074.VOR.pdf 2023-07-06T16:07:05.1485131 Output 2939162 application/pdf Version of Record true © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. Distributed under the terms of a Creative Commons Attribution 4.0 License (CC BY 4.0). true eng https://creativecommons.org/licenses/by/4.0/
title	Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning
spellingShingle	Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning Michael Allan Moritz Kuehnel
title_short	Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning
title_full	Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning
title_fullStr	Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning
title_full_unstemmed	Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning
title_sort	Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning
author_id_str_mv	b1f40243f0e1ee0ec5aa706601527f6a 210dbad181ce095d6f8bf2bd1d616d4e
author_id_fullname_str_mv	b1f40243f0e1ee0ec5aa706601527f6a_*_Michael Allan 210dbad181ce095d6f8bf2bd1d616d4e_*_Moritz Kuehnel
author	Michael Allan Moritz Kuehnel
author2	Michael Allan Thomas Pichon Jade A. McCune Christine Cavazza Alan Le Goff Moritz Kuehnel
format	Journal article
container_title	Angewandte Chemie International Edition
container_volume	62
container_issue	22
publishDate	2023
institution	Swansea University
issn	1433-7851 1521-3773
doi_str_mv	10.1002/anie.202219176
publisher	Wiley
college_str	Faculty of Science and Engineering
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department_str	School of Engineering and Applied Sciences - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
url	http://dx.doi.org/10.1002/anie.202219176
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description	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.
published_date	2023-05-22T16:08:37Z
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score	11.013686

Augmenting the Performance of Hydrogenase for Aerobic Photocatalytic Hydrogen Evolution via Solvent Tuning

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