Visible-Light-Promoted Iridium(III)-Catalyzed Acceptorless Dehydrogenation of N‑Heterocycles at Room Temperature
An effective visible-light-promoted iridium(III)-catalyzed hydrogen production from N-heterocycles is described. A single iridium complex constitutes the photocatalytic system playing a dual task, harvesting visible-light and facilitating C–H cleavage and H2 formation at room temperature and withou...
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| Published in | ACS catalysis Vol. 12; no. 10; pp. 6238 - 6245 |
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| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
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United States
American Chemical Society
20.05.2022
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| Abstract | An effective visible-light-promoted iridium(III)-catalyzed hydrogen production from N-heterocycles is described. A single iridium complex constitutes the photocatalytic system playing a dual task, harvesting visible-light and facilitating C–H cleavage and H2 formation at room temperature and without additives. The presence of a chelating C–N ligand combining a mesoionic carbene ligand along with an amido functionality in the IrIII complex is essential to attain the photocatalytic transformation. Furthermore, the IrIII complex is also an efficient catalyst for the thermal reverse process under mild conditions, positioning itself as a proficient candidate for liquid organic hydrogen carrier technologies (LOHCs). Mechanistic studies support a light-induced formation of H2 from the Ir–H intermediate as the operating mode of the iridium complex. |
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| AbstractList | An effective visible-light-promoted
iridium(III)-catalyzed hydrogen
production from N-heterocycles is described. A single iridium complex
constitutes the photocatalytic system playing a dual task, harvesting
visible-light and facilitating C–H cleavage and H
2
formation at room temperature and without additives. The presence
of a chelating C–N ligand combining a mesoionic carbene ligand
along with an amido functionality in the Ir
III
complex
is essential to attain the photocatalytic transformation. Furthermore,
the Ir
III
complex is also an efficient catalyst for the
thermal reverse process under mild conditions, positioning itself
as a proficient candidate for liquid organic hydrogen carrier technologies
(LOHCs). Mechanistic studies support a light-induced formation of
H
2
from the Ir–H intermediate as the operating mode
of the iridium complex. An effective visible-light-promoted iridium(III)-catalyzed hydrogen production from N-heterocycles is described. A single iridium complex constitutes the photocatalytic system playing a dual task, harvesting visible-light and facilitating C-H cleavage and H2 formation at room temperature and without additives. The presence of a chelating C-N ligand combining a mesoionic carbene ligand along with an amido functionality in the IrIII complex is essential to attain the photocatalytic transformation. Furthermore, the IrIII complex is also an efficient catalyst for the thermal reverse process under mild conditions, positioning itself as a proficient candidate for liquid organic hydrogen carrier technologies (LOHCs). Mechanistic studies support a light-induced formation of H2 from the Ir-H intermediate as the operating mode of the iridium complex.An effective visible-light-promoted iridium(III)-catalyzed hydrogen production from N-heterocycles is described. A single iridium complex constitutes the photocatalytic system playing a dual task, harvesting visible-light and facilitating C-H cleavage and H2 formation at room temperature and without additives. The presence of a chelating C-N ligand combining a mesoionic carbene ligand along with an amido functionality in the IrIII complex is essential to attain the photocatalytic transformation. Furthermore, the IrIII complex is also an efficient catalyst for the thermal reverse process under mild conditions, positioning itself as a proficient candidate for liquid organic hydrogen carrier technologies (LOHCs). Mechanistic studies support a light-induced formation of H2 from the Ir-H intermediate as the operating mode of the iridium complex. An effective visible-light-promoted iridium(III)-catalyzed hydrogen production from N-heterocycles is described. A single iridium complex constitutes the photocatalytic system playing a dual task, harvesting visible-light and facilitating C-H cleavage and H formation at room temperature and without additives. The presence of a chelating C-N ligand combining a mesoionic carbene ligand along with an amido functionality in the Ir complex is essential to attain the photocatalytic transformation. Furthermore, the Ir complex is also an efficient catalyst for the thermal reverse process under mild conditions, positioning itself as a proficient candidate for liquid organic hydrogen carrier technologies (LOHCs). Mechanistic studies support a light-induced formation of H from the Ir-H intermediate as the operating mode of the iridium complex. An effective visible-light-promoted iridium(III)-catalyzed hydrogen production from N-heterocycles is described. A single iridium complex constitutes the photocatalytic system playing a dual task, harvesting visible-light and facilitating C–H cleavage and H2 formation at room temperature and without additives. The presence of a chelating C–N ligand combining a mesoionic carbene ligand along with an amido functionality in the IrIII complex is essential to attain the photocatalytic transformation. Furthermore, the IrIII complex is also an efficient catalyst for the thermal reverse process under mild conditions, positioning itself as a proficient candidate for liquid organic hydrogen carrier technologies (LOHCs). Mechanistic studies support a light-induced formation of H2 from the Ir–H intermediate as the operating mode of the iridium complex. |
| Author | Mata, Jose A. Ibáñez-Ibáñez, Laura Guisado-Barrios, Gregorio Mejuto, Carmen |
| AuthorAffiliation | CSIC-Universidad de Zaragoza Institute of Advanced Materials (INAM), Centro de Innovación en Química Avanzada (ORFEO-CINQA) Departamento de Química Inorgánica. Instituto de Síntesis Química y Catálisis Homogénea (ISQCH) |
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| Author_xml | – sequence: 1 givenname: Carmen orcidid: 0000-0002-4432-5697 surname: Mejuto fullname: Mejuto, Carmen organization: Institute of Advanced Materials (INAM), Centro de Innovación en Química Avanzada (ORFEO-CINQA) – sequence: 2 givenname: Laura surname: Ibáñez-Ibáñez fullname: Ibáñez-Ibáñez, Laura organization: Institute of Advanced Materials (INAM), Centro de Innovación en Química Avanzada (ORFEO-CINQA) – sequence: 3 givenname: Gregorio orcidid: 0000-0002-0154-9682 surname: Guisado-Barrios fullname: Guisado-Barrios, Gregorio email: gguisado@unizar.es organization: CSIC-Universidad de Zaragoza – sequence: 4 givenname: Jose A. orcidid: 0000-0001-9310-2783 surname: Mata fullname: Mata, Jose A. email: jmata@uji.es organization: Institute of Advanced Materials (INAM), Centro de Innovación en Química Avanzada (ORFEO-CINQA) |
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| Keywords | iridium LOHCs dehydrogenation photocatalysis hydrogenation N-heterocycles hydrogen storage |
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| Snippet | An effective visible-light-promoted iridium(III)-catalyzed hydrogen production from N-heterocycles is described. A single iridium complex constitutes the... An effective visible-light-promoted iridium(III)-catalyzed hydrogen production from N-heterocycles is described. A single iridium complex constitutes the... An effective visible-light-promoted iridium(III)-catalyzed hydrogen production from N-heterocycles is described. A single iridium complex constitutes the... |
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| Title | Visible-Light-Promoted Iridium(III)-Catalyzed Acceptorless Dehydrogenation of N‑Heterocycles at Room Temperature |
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