Dinitrogen Cleavage and Hydrogenation by a Trinuclear Titanium Polyhydride Complex
Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N=N triple bond and forming an N-H bond. This has spurred investigations of the reactivity of molecular multimetallic hydrides with dinitrogen. We report here the re...
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| Published in | Science (American Association for the Advancement of Science) Vol. 340; no. 6140; pp. 1549 - 1552 |
|---|---|
| Main Authors | , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Washington, DC
American Association for the Advancement of Science
28.06.2013
The American Association for the Advancement of Science |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N=N triple bond and forming an N-H bond. This has spurred investigations of the reactivity of molecular multimetallic hydrides with dinitrogen. We report here the reaction of a trinuclear titanium polyhydride complex with dinitrogen, which induces dinitrogen cleavage and partial hydrogénation at ambient temperature and pressure. By ¹H and ¹⁵N nuclear magnetic resonance, x-ray crystallographic, and computational studies of some key reaction steps and products, we have determined that the dinitrogen (N₂) reduction proceeds sequentially through scission of a N₂ molecule bonded to three Ti atoms in a μ-η¹:η²:η²-end-on-side-on fashion to give a μ₂-N/μ₃-N dinitrido species, followed by intramolecular hydrogen migration from Ti to the μ₂-N nitrido unit. |
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| AbstractList | A century after its discovery, the Haber Bosch process is still used to produce ammonia from nitrogen for fertilizer. Nonetheless, the process requires high temperature and pressure, and chemists continue to look for synthetic analogs to microbial nitrogenase enzymes, which have managed to slice through the N2 triple bond under ambient conditions for millennia. Most efforts in this vein have relied on a boost from the reducing power of alkali metals. Shima et al. (p. 1549; see the Perspective by Fryzuk) instead explored the reactivity of a titanium hydride cluster, which cleanly slices through N2 at room temperature and incorporates the separated N atoms into its framework. Though ammonia was not produced, the system offers hope in the search for mild nitrogen reduction catalysts. [PUBLICATION ABSTRACT] Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N≡N triple bond and forming an N-H bond. This has spurred investigations of the reactivity of molecular multimetallic hydrides with dinitrogen. We report here the reaction of a trinuclear titanium polyhydride complex with dinitrogen, which induces dinitrogen cleavage and partial hydrogenation at ambient temperature and pressure. By 1H and 15N nuclear magnetic resonance, x-ray crystallographic, and computational studies of some key reaction steps and products, we have determined that the dinitrogen (N2) reduction proceeds sequentially through scission of a N2 molecule bonded to three Ti atoms in a μ-η1:η2:η2-end-on-side-on fashion to give a μ2-N/μ3-N dinitrido species, followed by intramolecular hydrogen migration from Ti to the μ2-N nitrido unit. [PUBLICATION ABSTRACT] Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N≡N triple bond and forming an N-H bond. This has spurred investigations of the reactivity of molecular multimetallic hydrides with dinitrogen. We report here the reaction of a trinuclear titanium polyhydride complex with dinitrogen, which induces dinitrogen cleavage and partial hydrogenation at ambient temperature and pressure. By (1)H and (15)N nuclear magnetic resonance, x-ray crystallographic, and computational studies of some key reaction steps and products, we have determined that the dinitrogen (N2) reduction proceeds sequentially through scission of a N2 molecule bonded to three Ti atoms in a μ-η(1):η(2):η(2)-end-on-side-on fashion to give a μ2-N/μ3-N dinitrido species, followed by intramolecular hydrogen migration from Ti to the μ2-N nitrido unit. Titanium Cleaver A century after its discovery, the Haber Bosch process is still used to produce ammonia from nitrogen for fertilizer. Nonetheless, the process requires high temperature and pressure, and chemists continue to look for synthetic analogs to microbial nitrogenase enzymes, which have managed to slice through the N2 triple bond under ambient conditions for millennia. Most efforts in this vein have relied on a boost from the reducing power of alkali metals. Shima et al. (p. 1549; see the Perspective by Fryzuk) instead explored the reactivity of a titanium hydride cluster, which cleanly slices through N ₂ at room temperature and incorporates the separated N atoms into its framework. Though ammonia was not produced, the system offers hope in the search for mild nitrogen reduction catalysts. Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N≡N triple bond and forming an N-H bond. This has spurred investigations of the reactivity of molecular multimetallic hydrides with dinitrogen. We report here the reaction of a trinuclear titanium polyhydride complex with dinitrogen, which induces dinitrogen cleavage and partial hydrogenation at ambient temperature and pressure. By (1)H and (15)N nuclear magnetic resonance, x-ray crystallographic, and computational studies of some key reaction steps and products, we have determined that the dinitrogen (N2) reduction proceeds sequentially through scission of a N2 molecule bonded to three Ti atoms in a μ-η(1):η(2):η(2)-end-on-side-on fashion to give a μ2-N/μ3-N dinitrido species, followed by intramolecular hydrogen migration from Ti to the μ2-N nitrido unit.Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N≡N triple bond and forming an N-H bond. This has spurred investigations of the reactivity of molecular multimetallic hydrides with dinitrogen. We report here the reaction of a trinuclear titanium polyhydride complex with dinitrogen, which induces dinitrogen cleavage and partial hydrogenation at ambient temperature and pressure. By (1)H and (15)N nuclear magnetic resonance, x-ray crystallographic, and computational studies of some key reaction steps and products, we have determined that the dinitrogen (N2) reduction proceeds sequentially through scission of a N2 molecule bonded to three Ti atoms in a μ-η(1):η(2):η(2)-end-on-side-on fashion to give a μ2-N/μ3-N dinitrido species, followed by intramolecular hydrogen migration from Ti to the μ2-N nitrido unit. Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N=N triple bond and forming an N-H bond. This has spurred investigations of the reactivity of molecular multimetallic hydrides with dinitrogen. We report here the reaction of a trinuclear titanium polyhydride complex with dinitrogen, which induces dinitrogen cleavage and partial hydrogénation at ambient temperature and pressure. By ¹H and ¹⁵N nuclear magnetic resonance, x-ray crystallographic, and computational studies of some key reaction steps and products, we have determined that the dinitrogen (N₂) reduction proceeds sequentially through scission of a N₂ molecule bonded to three Ti atoms in a μ-η¹:η²:η²-end-on-side-on fashion to give a μ₂-N/μ₃-N dinitrido species, followed by intramolecular hydrogen migration from Ti to the μ₂-N nitrido unit. Titanium CleaverA century after its discovery, the Haber Bosch process is still used to produce ammonia from nitrogen for fertilizer. Nonetheless, the process requires high temperature and pressure, and chemists continue to look for synthetic analogs to microbial nitrogenase enzymes, which have managed to slice through the N2 triple bond under ambient conditions for millennia. Most efforts in this vein have relied on a boost from the reducing power of alkali metals. Shima et al. (p. 1549; see the Perspective by Fryzuk) instead explored the reactivity of a titanium hydride cluster, which cleanly slices through N2 at room temperature and incorporates the separated N atoms into its framework. Though ammonia was not produced, the system offers hope in the search for mild nitrogen reduction catalysts. A century after its discovery, the Haber Bosch process is still used to produce ammonia from nitrogen for fertilizer. Nonetheless, the process requires high temperature and pressure, and chemists continue to look for synthetic analogs to microbial nitrogenase enzymes, which have managed to slice through the N2 triple bond under ambient conditions for millennia. Most efforts in this vein have relied on a boost from the reducing power of alkali metals. Shima et al. (p. 1549 ; see the Perspective by Fryzuk ) instead explored the reactivity of a titanium hydride cluster, which cleanly slices through N 2 at room temperature and incorporates the separated N atoms into its framework. Though ammonia was not produced, the system offers hope in the search for mild nitrogen reduction catalysts. The collective reactivity of three hydride-bridged titanium centers cleaves dinitrogen under mild conditions. [Also see Perspective by Fryzuk ] Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N≡N triple bond and forming an N–H bond. This has spurred investigations of the reactivity of molecular multimetallic hydrides with dinitrogen. We report here the reaction of a trinuclear titanium polyhydride complex with dinitrogen, which induces dinitrogen cleavage and partial hydrogenation at ambient temperature and pressure. By 1 H and 15 N nuclear magnetic resonance, x-ray crystallographic, and computational studies of some key reaction steps and products, we have determined that the dinitrogen (N 2 ) reduction proceeds sequentially through scission of a N 2 molecule bonded to three Ti atoms in a μ-η 1 :η 2 :η 2 -end-on-side-on fashion to give a μ 2 -N/μ 3 -N dinitrido species, followed by intramolecular hydrogen migration from Ti to the μ 2 -N nitrido unit. |
| Author | Hou, Zhaomin Kang, Xiaohui Hu, Shaowei Luo, Yi Shima, Takanori Luo, Gen |
| Author_xml | – sequence: 1 givenname: Takanori surname: Shima fullname: Shima, Takanori – sequence: 2 givenname: Shaowei surname: Hu fullname: Hu, Shaowei – sequence: 3 givenname: Gen surname: Luo fullname: Luo, Gen – sequence: 4 givenname: Xiaohui surname: Kang fullname: Kang, Xiaohui – sequence: 5 givenname: Yi surname: Luo fullname: Luo, Yi – sequence: 6 givenname: Zhaomin surname: Hou fullname: Hou, Zhaomin |
| BackLink | http://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=27784764$$DView record in Pascal Francis https://www.ncbi.nlm.nih.gov/pubmed/23812710$$D View this record in MEDLINE/PubMed |
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| Keywords | Titanium Complexes Transition element complexes Trinuclear complex Organometallic compound Enzymatic catalysis Activation Nitrogen Chemical reactivity Hydrogenation Chemical reaction kinetics Hydrido complex |
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| Snippet | Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N=N triple bond and... A century after its discovery, the Haber Bosch process is still used to produce ammonia from nitrogen for fertilizer. Nonetheless, the process requires high... Both the Haber-Bosch and biological ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong N≡N triple bond and... Titanium CleaverA century after its discovery, the Haber Bosch process is still used to produce ammonia from nitrogen for fertilizer. Nonetheless, the process... Titanium Cleaver A century after its discovery, the Haber Bosch process is still used to produce ammonia from nitrogen for fertilizer. Nonetheless, the process... |
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| Title | Dinitrogen Cleavage and Hydrogenation by a Trinuclear Titanium Polyhydride Complex |
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