Activation of dihydrogen and coordination of molecular H2 on transition metals
Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic c...
Ausführliche Beschreibung
Gespeichert in:
| Autor*in: |
Kubas, Gregory J. [verfasserIn] |
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| Format: |
E-Artikel |
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| Sprache: |
Englisch |
| Erschienen: |
2014transfer abstract |
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| Umfang: |
17 |
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| Übergeordnetes Werk: |
Enthalten in: The Effect of Simultaneous Renal Replacement Therapy on Extracorporeal Membrane Oxygenation Support for Postcardiotomy Patients with Cardiogenic Shock: A Pilot Randomized Controlled Trial - Li, Chenglong ELSEVIER, 2019, New York, NY [u.a.] |
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| Übergeordnetes Werk: |
volume:751 ; year:2014 ; day:1 ; month:02 ; pages:33-49 ; extent:17 |
| Links: |
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| DOI / URN: |
10.1016/j.jorganchem.2013.07.041 |
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| 520 | |a Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. | ||
| 520 | |a Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. | ||
| 650 | 7 | |a Hydrogen storage |2 Elsevier | |
| 650 | 7 | |a Biomimetic hydrogen production |2 Elsevier | |
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| 650 | 7 | |a Hydrogen activation |2 Elsevier | |
| 650 | 7 | |a Dihydrogen complex |2 Elsevier | |
| 650 | 7 | |a Sigma bond complex |2 Elsevier | |
| 773 | 0 | 8 | |i Enthalten in |n Elsevier |a Li, Chenglong ELSEVIER |t The Effect of Simultaneous Renal Replacement Therapy on Extracorporeal Membrane Oxygenation Support for Postcardiotomy Patients with Cardiogenic Shock: A Pilot Randomized Controlled Trial |d 2019 |g New York, NY [u.a.] |w (DE-627)ELV002971518 |
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10.1016/j.jorganchem.2013.07.041 doi GBVA2014022000004.pica (DE-627)ELV028509196 (ELSEVIER)S0022-328X(13)00548-2 DE-627 ger DE-627 rakwb eng 540 540 DE-600 610 VZ 44.85 bkl 44.66 bkl Kubas, Gregory J. verfasserin aut Activation of dihydrogen and coordination of molecular H2 on transition metals 2014transfer abstract 17 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Hydrogen storage Elsevier Biomimetic hydrogen production Elsevier Alkane complex Elsevier Hydrogen activation Elsevier Dihydrogen complex Elsevier Sigma bond complex Elsevier Enthalten in Elsevier Li, Chenglong ELSEVIER The Effect of Simultaneous Renal Replacement Therapy on Extracorporeal Membrane Oxygenation Support for Postcardiotomy Patients with Cardiogenic Shock: A Pilot Randomized Controlled Trial 2019 New York, NY [u.a.] (DE-627)ELV002971518 volume:751 year:2014 day:1 month:02 pages:33-49 extent:17 https://doi.org/10.1016/j.jorganchem.2013.07.041 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA 44.85 Kardiologie Angiologie VZ 44.66 Anästhesiologie VZ AR 751 2014 1 0201 33-49 17 045F 540 |
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10.1016/j.jorganchem.2013.07.041 doi GBVA2014022000004.pica (DE-627)ELV028509196 (ELSEVIER)S0022-328X(13)00548-2 DE-627 ger DE-627 rakwb eng 540 540 DE-600 610 VZ 44.85 bkl 44.66 bkl Kubas, Gregory J. verfasserin aut Activation of dihydrogen and coordination of molecular H2 on transition metals 2014transfer abstract 17 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Hydrogen storage Elsevier Biomimetic hydrogen production Elsevier Alkane complex Elsevier Hydrogen activation Elsevier Dihydrogen complex Elsevier Sigma bond complex Elsevier Enthalten in Elsevier Li, Chenglong ELSEVIER The Effect of Simultaneous Renal Replacement Therapy on Extracorporeal Membrane Oxygenation Support for Postcardiotomy Patients with Cardiogenic Shock: A Pilot Randomized Controlled Trial 2019 New York, NY [u.a.] (DE-627)ELV002971518 volume:751 year:2014 day:1 month:02 pages:33-49 extent:17 https://doi.org/10.1016/j.jorganchem.2013.07.041 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA 44.85 Kardiologie Angiologie VZ 44.66 Anästhesiologie VZ AR 751 2014 1 0201 33-49 17 045F 540 |
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10.1016/j.jorganchem.2013.07.041 doi GBVA2014022000004.pica (DE-627)ELV028509196 (ELSEVIER)S0022-328X(13)00548-2 DE-627 ger DE-627 rakwb eng 540 540 DE-600 610 VZ 44.85 bkl 44.66 bkl Kubas, Gregory J. verfasserin aut Activation of dihydrogen and coordination of molecular H2 on transition metals 2014transfer abstract 17 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Hydrogen storage Elsevier Biomimetic hydrogen production Elsevier Alkane complex Elsevier Hydrogen activation Elsevier Dihydrogen complex Elsevier Sigma bond complex Elsevier Enthalten in Elsevier Li, Chenglong ELSEVIER The Effect of Simultaneous Renal Replacement Therapy on Extracorporeal Membrane Oxygenation Support for Postcardiotomy Patients with Cardiogenic Shock: A Pilot Randomized Controlled Trial 2019 New York, NY [u.a.] (DE-627)ELV002971518 volume:751 year:2014 day:1 month:02 pages:33-49 extent:17 https://doi.org/10.1016/j.jorganchem.2013.07.041 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA 44.85 Kardiologie Angiologie VZ 44.66 Anästhesiologie VZ AR 751 2014 1 0201 33-49 17 045F 540 |
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10.1016/j.jorganchem.2013.07.041 doi GBVA2014022000004.pica (DE-627)ELV028509196 (ELSEVIER)S0022-328X(13)00548-2 DE-627 ger DE-627 rakwb eng 540 540 DE-600 610 VZ 44.85 bkl 44.66 bkl Kubas, Gregory J. verfasserin aut Activation of dihydrogen and coordination of molecular H2 on transition metals 2014transfer abstract 17 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Hydrogen storage Elsevier Biomimetic hydrogen production Elsevier Alkane complex Elsevier Hydrogen activation Elsevier Dihydrogen complex Elsevier Sigma bond complex Elsevier Enthalten in Elsevier Li, Chenglong ELSEVIER The Effect of Simultaneous Renal Replacement Therapy on Extracorporeal Membrane Oxygenation Support for Postcardiotomy Patients with Cardiogenic Shock: A Pilot Randomized Controlled Trial 2019 New York, NY [u.a.] (DE-627)ELV002971518 volume:751 year:2014 day:1 month:02 pages:33-49 extent:17 https://doi.org/10.1016/j.jorganchem.2013.07.041 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA 44.85 Kardiologie Angiologie VZ 44.66 Anästhesiologie VZ AR 751 2014 1 0201 33-49 17 045F 540 |
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10.1016/j.jorganchem.2013.07.041 doi GBVA2014022000004.pica (DE-627)ELV028509196 (ELSEVIER)S0022-328X(13)00548-2 DE-627 ger DE-627 rakwb eng 540 540 DE-600 610 VZ 44.85 bkl 44.66 bkl Kubas, Gregory J. verfasserin aut Activation of dihydrogen and coordination of molecular H2 on transition metals 2014transfer abstract 17 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. Hydrogen storage Elsevier Biomimetic hydrogen production Elsevier Alkane complex Elsevier Hydrogen activation Elsevier Dihydrogen complex Elsevier Sigma bond complex Elsevier Enthalten in Elsevier Li, Chenglong ELSEVIER The Effect of Simultaneous Renal Replacement Therapy on Extracorporeal Membrane Oxygenation Support for Postcardiotomy Patients with Cardiogenic Shock: A Pilot Randomized Controlled Trial 2019 New York, NY [u.a.] (DE-627)ELV002971518 volume:751 year:2014 day:1 month:02 pages:33-49 extent:17 https://doi.org/10.1016/j.jorganchem.2013.07.041 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA 44.85 Kardiologie Angiologie VZ 44.66 Anästhesiologie VZ AR 751 2014 1 0201 33-49 17 045F 540 |
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Enthalten in The Effect of Simultaneous Renal Replacement Therapy on Extracorporeal Membrane Oxygenation Support for Postcardiotomy Patients with Cardiogenic Shock: A Pilot Randomized Controlled Trial New York, NY [u.a.] volume:751 year:2014 day:1 month:02 pages:33-49 extent:17 |
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Activation of dihydrogen and coordination of molecular H2 on transition metals |
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Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. |
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Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. |
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Fifty years ago, when this journal was founded, organometallic chemists could not have imagined that common small molecules such as dinitrogen and especially dihydrogen could function as ligands. Dihydrogen has long been vital in catalytic processes such as hydrogenation and conversions of organic compounds and is now being considered as a future energy storage medium. Dihydrogen is only useful chemically when the two strongly bound H atoms are split apart in a controlled fashion. Although metal hydrides were first well established in 1955, the structure and mechanism by which H2 binds to and undergoes cleavage on transition metals was not ascertained until even more recently in the history of inorganometallic chemistry, about 20 years after this journal was first published. The activation of dihydrogen is a fascinating saga that has slowly unfolded over the past 80+ years, as will be chronicled in this Perspective. There is a marvelous analogy between the metal-olefin π bonding model first brought to light by Dewar, Chatt, and Duncanson 60 years ago and the bonding model for side-on σ-bond coordination discovered by us 30 years ago. There are two separate pathways for H–H (and X–H σ-bond activation in general) that directly depend on the electronics of the metal σ-ligand bonding. Metal d to σ* X–H backdonation is the key to stabilizing σ-bond coordination and also is crucial to its homolytic cleavage (oxidation addition). For electrophilic complexes, particularly cationic systems with minimal backdonation, heterolytic cleavage of H2 is common and is a key reaction in industrial and biological catalysis. |
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