Dinitrogen Activation by Heteronuclear Metal Carbide Cluster Anions FeTaC2- : A 5d Early and 3d Late Transition Metal Strategy
Cleavage of the strong N≡N bond has long been a great challenge for energy-efficient dinitrogen (N2) fixation; thus a reasonable design of reactive species to activate N2 under mild conditions is highly desirable and meaningful. Herein a novel N2 activation strategy of combining 5d early (E) and 3d late (L) transition metals (TMs) is proposed, which is verified by the facile and complete N≡N cleavage via the polarized Fe-Ta bond in gas-phase cluster FeTaC2-. The efficient N≡N cleavage benefits from an electronic-level design of highly strengthened donor-acceptor interactions, in which the 5d-ETM (Ta) mainly pushes electrons from occupied 5d-orbitals to N2 π*-orbitals while the 3d-LTM (Fe) simultaneously pulls electrons from N2 σ/π-orbitals to its unoccupied 3d-orbitals. Through employing 5d-ETM and 3d-LTM to play their respective roles, this work provides a new and versatile idea for activating the inert N≡N bond and inspires relevant design of TM-based catalysts.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2021 |
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| Erschienen: |
2021 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:143 |
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| Enthalten in: |
Journal of the American Chemical Society - 143(2021), 45 vom: 17. Nov., Seite 19224-19231 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Mou, Li-Hui [VerfasserIn] |
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| Links: |
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| Anmerkungen: |
Date Revised 17.11.2021 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1021/jacs.1c10018 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM332696928 |
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| 245 | 1 | 0 | |a Dinitrogen Activation by Heteronuclear Metal Carbide Cluster Anions FeTaC2- |b A 5d Early and 3d Late Transition Metal Strategy |
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| 500 | |a Date Revised 17.11.2021 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Cleavage of the strong N≡N bond has long been a great challenge for energy-efficient dinitrogen (N2) fixation; thus a reasonable design of reactive species to activate N2 under mild conditions is highly desirable and meaningful. Herein a novel N2 activation strategy of combining 5d early (E) and 3d late (L) transition metals (TMs) is proposed, which is verified by the facile and complete N≡N cleavage via the polarized Fe-Ta bond in gas-phase cluster FeTaC2-. The efficient N≡N cleavage benefits from an electronic-level design of highly strengthened donor-acceptor interactions, in which the 5d-ETM (Ta) mainly pushes electrons from occupied 5d-orbitals to N2 π*-orbitals while the 3d-LTM (Fe) simultaneously pulls electrons from N2 σ/π-orbitals to its unoccupied 3d-orbitals. Through employing 5d-ETM and 3d-LTM to play their respective roles, this work provides a new and versatile idea for activating the inert N≡N bond and inspires relevant design of TM-based catalysts | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Li, Yao |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Zi-Yu |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Qing-Yu |e verfasserin |4 aut | |
| 700 | 1 | |a Chen, Hui |e verfasserin |4 aut | |
| 700 | 1 | |a He, Sheng-Gui |e verfasserin |4 aut | |
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