One-pot, room-temperature conversion of dinitrogen to ammonium chloride at a main-group element

被引:98
作者
Legare, Marc-Andre [1 ,2 ,3 ]
Belanger-Chabot, Guillaume [1 ,2 ,4 ]
Rang, Maximilian [1 ,2 ]
Dewhurst, Rian D. [1 ,2 ]
Krummenacher, Ivo [1 ,2 ]
Bertermann, Ruediger [1 ,2 ]
Braunschweig, Holger [1 ,2 ]
机构
[1] Julius Maximilians Univ Wurzburg, Inst Inorgan Chem, Wurzburg, Germany
[2] Julius Maximilians Univ Wurzburg, Inst Sustainable Chem & Catalysis Boron, Wurzburg, Germany
[3] McGill Univ, Dept Chem, Montreal, PQ, Canada
[4] Univ Laval, Dept Chim, Quebec City, PQ, Canada
基金
加拿大自然科学与工程研究理事会;
关键词
NITROGEN-FIXATION; N-2; REDUCTION; CHEMISTRY; CLEAVAGE; HYDROGENATION; COMPLEXES; CARBENES; CO;
D O I
10.1038/s41557-020-0520-6
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The industrial reduction of dinitrogen (N-2) to ammonia is an energy-intensive process that consumes a considerable proportion of the global energy supply. As a consequence, species that can bind N-2 and cleave its strong N-N bond under mild conditions have been sought for decades. Until recently, the only species known to support N-2 fixation and functionalization were based on a handful of metals of thesanddblocks of the periodic table. Here we present one-pot binding, cleavage and reduction of N-2 to ammonium by a main-group species. The reaction-a complex multiple reduction-protonation sequence-proceeds at room temperature in a single synthetic step through the use of solid-phase reductant and acid reagents. A simple acid quench of the mixture then provides ammonium, the protonated form of ammonia present in fertilizer. The elementary reaction steps in the process are elucidated, including the crucial N-N bond cleavage process, and all of the intermediates of the reaction are isolated.
引用
收藏
页码:1076 / 1080
页数:8
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