Artificial Hydrogenases Based on Cobaloximes and Heme Oxygenase
International audience The insertion of cobaloxime catalysts in the heme-binding pocket of heme oxygenase (HO) yields artificial hydrogenases active for H-2 evolution in neutral aqueous solutions. These novel biohybrids have been purified and characterized by using UV/visible and EPR spectroscopy. T...
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ftceafr:oai:HAL:hal-01437557v1 2024-09-15T18:37:34+00:00 Artificial Hydrogenases Based on Cobaloximes and Heme Oxygenase Bacchi, Marine Veinberg, Elias Field, Martin J Niklas, Jens Matsui, Toshitaka Tiede, David M. Poluektov, Oleg G. Ikeda-Saito, Masao Fontecave, Marc Artero, Vincent Laboratoire de Chimie et Biologie des Métaux (LCBM - UMR 5249) Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut de Recherche Interdisciplinaire de Grenoble (IRIG) Direction de Recherche Fondamentale (CEA) (DRF (CEA)) Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)) Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA) Institut de biologie structurale (IBS - UMR 5075 ) Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut de Recherche Interdisciplinaire de Grenoble (IRIG) Argonne National Laboratory Lemont (ANL) Institute of Multidisciplinary Research for Advanced Materials Tohoku University Sendai Collège de France - Chaire Chimie des processus biologiques Laboratoire de Chimie des Processus Biologiques (LCPB) Collège de France (CdF (institution))-Institut de Chimie - CNRS Chimie (INC-CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Institut de Chimie - CNRS Chimie (INC-CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS) ANR-11-LABX-0003,ARCANE,Grenoble, une chimie bio-motivée(2011) 2016-10 https://hal.science/hal-01437557 https://doi.org/10.1002/cplu.201600218 en eng HAL CCSD Wiley info:eu-repo/semantics/altIdentifier/doi/10.1002/cplu.201600218 hal-01437557 https://hal.science/hal-01437557 doi:10.1002/cplu.201600218 ISSN: 2192-6506 ChemPlusChem https://hal.science/hal-01437557 ChemPlusChem, 2016, 81 (10 Spécial issue), pp.1083-1089. ⟨10.1002/cplu.201600218⟩ biohybrids cobalt heme proteins enzyme models hydrogen evolution [CHIM]Chemical Sciences [CHIM.CATA]Chemical Sciences/Catalysis info:eu-repo/semantics/article Journal articles 2016 ftceafr https://doi.org/10.1002/cplu.201600218 2024-07-22T13:29:33Z International audience The insertion of cobaloxime catalysts in the heme-binding pocket of heme oxygenase (HO) yields artificial hydrogenases active for H-2 evolution in neutral aqueous solutions. These novel biohybrids have been purified and characterized by using UV/visible and EPR spectroscopy. These analyses revealed the presence of two distinct binding conformations, thereby providing the cobaloxime with hydrophobic and hydrophilic environments, respectively. Quantum chemical/molecular mechanical docking calculations found open and closed conformations of the binding pocket owing to mobile amino acid residues. HO-based biohybrids incorporating a {Co(dmgH)(2)} (dmgH(2)=dimethylglyoxime) catalytic center displayed up to threefold increased turnover numbers with respect to the cobaloxime alone or to analogous sperm whale myoglobin adducts. This study thus provides a strong basis for further improvement of such biohybrids, using well-designed modifications of the second and outer coordination spheres, through site-directed mutagenesis of the host protein. Article in Journal/Newspaper Sperm whale HAL-CEA (Commissariat à l'énergie atomique et aux énergies alternatives) ChemPlusChem 81 10 1083 1089 |
institution |
Open Polar |
collection |
HAL-CEA (Commissariat à l'énergie atomique et aux énergies alternatives) |
op_collection_id |
ftceafr |
language |
English |
topic |
biohybrids cobalt heme proteins enzyme models hydrogen evolution [CHIM]Chemical Sciences [CHIM.CATA]Chemical Sciences/Catalysis |
spellingShingle |
biohybrids cobalt heme proteins enzyme models hydrogen evolution [CHIM]Chemical Sciences [CHIM.CATA]Chemical Sciences/Catalysis Bacchi, Marine Veinberg, Elias Field, Martin J Niklas, Jens Matsui, Toshitaka Tiede, David M. Poluektov, Oleg G. Ikeda-Saito, Masao Fontecave, Marc Artero, Vincent Artificial Hydrogenases Based on Cobaloximes and Heme Oxygenase |
topic_facet |
biohybrids cobalt heme proteins enzyme models hydrogen evolution [CHIM]Chemical Sciences [CHIM.CATA]Chemical Sciences/Catalysis |
description |
International audience The insertion of cobaloxime catalysts in the heme-binding pocket of heme oxygenase (HO) yields artificial hydrogenases active for H-2 evolution in neutral aqueous solutions. These novel biohybrids have been purified and characterized by using UV/visible and EPR spectroscopy. These analyses revealed the presence of two distinct binding conformations, thereby providing the cobaloxime with hydrophobic and hydrophilic environments, respectively. Quantum chemical/molecular mechanical docking calculations found open and closed conformations of the binding pocket owing to mobile amino acid residues. HO-based biohybrids incorporating a {Co(dmgH)(2)} (dmgH(2)=dimethylglyoxime) catalytic center displayed up to threefold increased turnover numbers with respect to the cobaloxime alone or to analogous sperm whale myoglobin adducts. This study thus provides a strong basis for further improvement of such biohybrids, using well-designed modifications of the second and outer coordination spheres, through site-directed mutagenesis of the host protein. |
author2 |
Laboratoire de Chimie et Biologie des Métaux (LCBM - UMR 5249) Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut de Recherche Interdisciplinaire de Grenoble (IRIG) Direction de Recherche Fondamentale (CEA) (DRF (CEA)) Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)) Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA) Institut de biologie structurale (IBS - UMR 5075 ) Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut de Recherche Interdisciplinaire de Grenoble (IRIG) Argonne National Laboratory Lemont (ANL) Institute of Multidisciplinary Research for Advanced Materials Tohoku University Sendai Collège de France - Chaire Chimie des processus biologiques Laboratoire de Chimie des Processus Biologiques (LCPB) Collège de France (CdF (institution))-Institut de Chimie - CNRS Chimie (INC-CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Institut de Chimie - CNRS Chimie (INC-CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS) ANR-11-LABX-0003,ARCANE,Grenoble, une chimie bio-motivée(2011) |
format |
Article in Journal/Newspaper |
author |
Bacchi, Marine Veinberg, Elias Field, Martin J Niklas, Jens Matsui, Toshitaka Tiede, David M. Poluektov, Oleg G. Ikeda-Saito, Masao Fontecave, Marc Artero, Vincent |
author_facet |
Bacchi, Marine Veinberg, Elias Field, Martin J Niklas, Jens Matsui, Toshitaka Tiede, David M. Poluektov, Oleg G. Ikeda-Saito, Masao Fontecave, Marc Artero, Vincent |
author_sort |
Bacchi, Marine |
title |
Artificial Hydrogenases Based on Cobaloximes and Heme Oxygenase |
title_short |
Artificial Hydrogenases Based on Cobaloximes and Heme Oxygenase |
title_full |
Artificial Hydrogenases Based on Cobaloximes and Heme Oxygenase |
title_fullStr |
Artificial Hydrogenases Based on Cobaloximes and Heme Oxygenase |
title_full_unstemmed |
Artificial Hydrogenases Based on Cobaloximes and Heme Oxygenase |
title_sort |
artificial hydrogenases based on cobaloximes and heme oxygenase |
publisher |
HAL CCSD |
publishDate |
2016 |
url |
https://hal.science/hal-01437557 https://doi.org/10.1002/cplu.201600218 |
genre |
Sperm whale |
genre_facet |
Sperm whale |
op_source |
ISSN: 2192-6506 ChemPlusChem https://hal.science/hal-01437557 ChemPlusChem, 2016, 81 (10 Spécial issue), pp.1083-1089. ⟨10.1002/cplu.201600218⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.1002/cplu.201600218 hal-01437557 https://hal.science/hal-01437557 doi:10.1002/cplu.201600218 |
op_doi |
https://doi.org/10.1002/cplu.201600218 |
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ChemPlusChem |
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81 |
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10 |
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1083 |
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1089 |
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1810481933962969088 |