The reductive coupling of dinitrogen

被引:215
作者
Legare, Marc-Andre [1 ,2 ]
Rang, Maximilian [1 ,2 ]
Belanger-Chabot, Guillaume [1 ,2 ]
Schweizer, Julia I. [3 ]
Krummenacher, Ivo [1 ,2 ]
Bertermann, Rudiger [1 ,2 ]
Arrowsmith, Merle [1 ,2 ]
Holthausen, Max C. [3 ]
Braunschweig, Holger [1 ,2 ]
机构
[1] Julius Maximilians Univ Wurzburg, Inst Inorgan Chem, D-97074 Wurzburg, Germany
[2] Julius Maximilians Univ Wurzburg, Inst Sustainable Chem & Catalysis Boron, D-97074 Wurzburg, Germany
[3] Goethe Univ, Inst Inorgan & Analyt Chem, Max von Laue Str 7, D-60438 Frankfurt, Germany
基金
加拿大自然科学与工程研究理事会;
关键词
STATE PERTURBATION-THEORY; GAUSSIAN-BASIS SETS; DIRADICAL CHARACTER; CRYSTAL-STRUCTURE; HIGH-PRESSURE; HARTREE-FOCK; NITROGEN; CHEMISTRY; DENSITY; ENERGY;
D O I
10.1126/science.aav9593
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The coupling of two or more molecules of dinitrogen (N-2) occurs naturally under the radiative conditions present in the ionosphere and may be achieved synthetically under ultrahigh pressure or plasma conditions. However, the comparatively low N-N single-bond enthalpy generally renders the catenation of the strongly triple-bonded N-2 diatomic unfavorable and the decomposition of nitrogen chains a common reaction motif. Here, we report the surprising organoboron-mediated catenation of two N-2 molecules under near-ambient conditions to form a complex in which a [N-4](2-) chain bridges two boron centers. The reaction entails reductive coupling of two hypovalent-boron-bound N-2 units in a single step. Both this complex and a derivative protonated at both ends of the chain were characterized crystallographically.
引用
收藏
页码:1329 / +
页数:78
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