A Non-Heme Diiron Complex for (Electro)catalytic Reduction of Dioxygen: Tuning the Selectivity through Electron Delivery
In the oxygen reduction reaction (ORR) domain, the investigation of new homogeneous catalysts is a crucial step toward the full comprehension of the key structural and/or electronic factors that control catalytic efficiency and selectivity. Herein, we report a unique non-heme diiron complex that can...
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| Published in | Journal of the American Chemical Society Vol. 141; no. 20; pp. 8244 - 8253 |
|---|---|
| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
22.05.2019
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0002-7863 1520-5126 1520-5126 |
| DOI | 10.1021/jacs.9b02011 |
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| Abstract | In the oxygen reduction reaction (ORR) domain, the investigation of new homogeneous catalysts is a crucial step toward the full comprehension of the key structural and/or electronic factors that control catalytic efficiency and selectivity. Herein, we report a unique non-heme diiron complex that can act as a homogeneous ORR catalyst in acetonitrile solution. This iron(II) thiolate dinuclear complex, [FeII 2(LS)(LSH)] ([Fe 2 SH ] + ) (LS2– = 2,2′-(2,2′-bipyridine-6,6′-diyl)bis(1,1-diphenylethanethiolate)) contains a thiol group in the metal coordination sphere. [Fe 2 SH ] + is an efficient ORR catalyst both in the presence of a one-electron reducing agent and under electrochemically assisted conditions. However, its selectivity is dependent on the electron delivery pathway; in particular, the process is selective for H2O2 production under chemical conditions (up to ∼95%), whereas H2O is the main product during electrocatalysis (less than ∼10% H2O2). Based on computational work alongside the experimental data, a mechanistic proposal is discussed that rationalizes the selective and tunable reduction of dioxygen. |
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| AbstractList | In the oxygen reduction reaction (ORR) domain, the investigation of new homogeneous catalysts is a crucial step toward the full comprehension of the key structural and/or electronic factors that control catalytic efficiency and selectivity. Herein, we report a unique non-heme diiron complex that can act as a homogeneous ORR catalyst in acetonitrile solution. This iron(II) thiolate dinuclear complex, [FeII2(LS)(LSH)] ([Fe2SH]+) (LS2- = 2,2'-(2,2'-bipyridine-6,6'-diyl)bis(1,1-diphenylethanethiolate)) contains a thiol group in the metal coordination sphere. [Fe2SH]+ is an efficient ORR catalyst both in the presence of a one-electron reducing agent and under electrochemically assisted conditions. However, its selectivity is dependent on the electron delivery pathway; in particular, the process is selective for H2O2 production under chemical conditions (up to ∼95%), whereas H2O is the main product during electrocatalysis (less than ∼10% H2O2). Based on computational work alongside the experimental data, a mechanistic proposal is discussed that rationalizes the selective and tunable reduction of dioxygen.In the oxygen reduction reaction (ORR) domain, the investigation of new homogeneous catalysts is a crucial step toward the full comprehension of the key structural and/or electronic factors that control catalytic efficiency and selectivity. Herein, we report a unique non-heme diiron complex that can act as a homogeneous ORR catalyst in acetonitrile solution. This iron(II) thiolate dinuclear complex, [FeII2(LS)(LSH)] ([Fe2SH]+) (LS2- = 2,2'-(2,2'-bipyridine-6,6'-diyl)bis(1,1-diphenylethanethiolate)) contains a thiol group in the metal coordination sphere. [Fe2SH]+ is an efficient ORR catalyst both in the presence of a one-electron reducing agent and under electrochemically assisted conditions. However, its selectivity is dependent on the electron delivery pathway; in particular, the process is selective for H2O2 production under chemical conditions (up to ∼95%), whereas H2O is the main product during electrocatalysis (less than ∼10% H2O2). Based on computational work alongside the experimental data, a mechanistic proposal is discussed that rationalizes the selective and tunable reduction of dioxygen. In the oxygen reduction reaction (ORR) domain, the investigation of new homogeneous catalysts is a crucial step toward the full comprehension of the key structural and/or electronic factors that control catalytic efficiency and selectivity. Herein, we report a unique non-heme diiron complex that can act as a homogeneous ORR catalyst in acetonitrile solution. This iron(II) thiolate dinuclear complex, [Fe (LS)(LSH)] ([Fe ] ) (LS = 2,2'-(2,2'-bipyridine-6,6'-diyl)bis(1,1-diphenylethanethiolate)) contains a thiol group in the metal coordination sphere. [Fe ] is an efficient ORR catalyst both in the presence of a one-electron reducing agent and under electrochemically assisted conditions. However, its selectivity is dependent on the electron delivery pathway; in particular, the process is selective for H O production under chemical conditions (up to ∼95%), whereas H O is the main product during electrocatalysis (less than ∼10% H O ). Based on computational work alongside the experimental data, a mechanistic proposal is discussed that rationalizes the selective and tunable reduction of dioxygen. In the oxygen reduction reaction (ORR) domain, the investigation of new homogeneous catalysts is a crucial step toward the full comprehension of the key structural and/or electronic factors that control catalytic efficiency and selectivity. Herein, we report a unique non-heme diiron complex that can act as a homogeneous ORR catalyst in acetonitrile solution. This iron(II) thiolate dinuclear complex, [FeII 2(LS)(LSH)] ([Fe 2 SH ] + ) (LS2– = 2,2′-(2,2′-bipyridine-6,6′-diyl)bis(1,1-diphenylethanethiolate)) contains a thiol group in the metal coordination sphere. [Fe 2 SH ] + is an efficient ORR catalyst both in the presence of a one-electron reducing agent and under electrochemically assisted conditions. However, its selectivity is dependent on the electron delivery pathway; in particular, the process is selective for H2O2 production under chemical conditions (up to ∼95%), whereas H2O is the main product during electrocatalysis (less than ∼10% H2O2). Based on computational work alongside the experimental data, a mechanistic proposal is discussed that rationalizes the selective and tunable reduction of dioxygen. In the Oxygen Reduction Reaction (ORR) domain, the investigation of new homogeneous catalysts is a crucial step towards the full comprehension of the key structural and/or electronic factors that control catalytic efficiency and selectivity. Herein, we report a unique non-heme diiron complex that can act as a homogeneous ORR catalyst in acetonitrile solution. This iron(II)-thiolate dinuclear complex, [FeII2(LS)(LSH)] ([Fe2SH]+) (LS2- = 2,2'-(2,2'-bipyridine-6,6'-diyl)bis(1,1-diphenylethanethiolate)) contains a thiol group in the metal coordination sphere. [Fe2SH]+ is an efficient ORR catalyst both in the presence of a one-electron reducing agent as well as under electrochemically assisted conditions. However, its selectivity is dependent on the electron delivery pathway, in particular, the process is selective for H2O2 production under chemical conditions (up to ~95%), whereas H2O is the main product during electrocatalysis (less than ~10% H2O2). Based on computational work alongside the experimental data, a mechanistic proposal is discussed that rationalizes the selective and tunable reduction of dioxygen. |
| Author | Wang, Lianke Philouze, Christian Gennari, Marcello Morozan, Adina Demeshko, Serhiy Artero, Vincent Duboc, Carole Cantú Reinhard, Fabián G Meyer, Franc de Visser, Sam P Gutiérrez, Javier |
| AuthorAffiliation | Institut für Anorganische Chemie Manchester Institute of Biotechnology and School of Chemical Engineering and Analytical Science Université Grenoble Alpes |
| AuthorAffiliation_xml | – name: Université Grenoble Alpes – name: Manchester Institute of Biotechnology and School of Chemical Engineering and Analytical Science – name: Institut für Anorganische Chemie |
| Author_xml | – sequence: 1 givenname: Lianke surname: Wang fullname: Wang, Lianke – sequence: 2 givenname: Marcello orcidid: 0000-0001-5205-1123 surname: Gennari fullname: Gennari, Marcello email: marcello.gennari@univ-grenoble-alpes.fr – sequence: 3 givenname: Fabián G surname: Cantú Reinhard fullname: Cantú Reinhard, Fabián G organization: Manchester Institute of Biotechnology and School of Chemical Engineering and Analytical Science – sequence: 4 givenname: Javier surname: Gutiérrez fullname: Gutiérrez, Javier – sequence: 5 givenname: Adina surname: Morozan fullname: Morozan, Adina organization: Université Grenoble Alpes – sequence: 6 givenname: Christian surname: Philouze fullname: Philouze, Christian – sequence: 7 givenname: Serhiy surname: Demeshko fullname: Demeshko, Serhiy organization: Institut für Anorganische Chemie – sequence: 8 givenname: Vincent orcidid: 0000-0002-6148-8471 surname: Artero fullname: Artero, Vincent organization: Université Grenoble Alpes – sequence: 9 givenname: Franc orcidid: 0000-0002-8613-7862 surname: Meyer fullname: Meyer, Franc organization: Institut für Anorganische Chemie – sequence: 10 givenname: Sam P orcidid: 0000-0002-2620-8788 surname: de Visser fullname: de Visser, Sam P email: sam.devisser@manchester.ac.uk organization: Manchester Institute of Biotechnology and School of Chemical Engineering and Analytical Science – sequence: 11 givenname: Carole orcidid: 0000-0002-9415-198X surname: Duboc fullname: Duboc, Carole email: carole.duboc@univ-grenoble-alpes.fr |
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| Snippet | In the oxygen reduction reaction (ORR) domain, the investigation of new homogeneous catalysts is a crucial step toward the full comprehension of the key... In the Oxygen Reduction Reaction (ORR) domain, the investigation of new homogeneous catalysts is a crucial step towards the full comprehension of the key... |
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| SubjectTerms | Catalysis Chemical Sciences |
| Title | A Non-Heme Diiron Complex for (Electro)catalytic Reduction of Dioxygen: Tuning the Selectivity through Electron Delivery |
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