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One-pot, room-temperature conversion of dinitrogen to ammonium chloride at a main-group element.
Nature Chemistry ( IF 19.2 ) Pub Date : 2020-09-14 , DOI: 10.1038/s41557-020-0520-6
Marc-André Légaré 1, 2, 3 , Guillaume Bélanger-Chabot 1, 2, 4 , Maximilian Rang 1, 2 , Rian D Dewhurst 1, 2 , Ivo Krummenacher 1, 2 , Rüdiger Bertermann 1, 2 , Holger Braunschweig 1, 2
Affiliation  

The industrial reduction of dinitrogen (N2) to ammonia is an energy-intensive process that consumes a considerable proportion of the global energy supply. As a consequence, species that can bind N2 and cleave its strong N–N bond under mild conditions have been sought for decades. Until recently, the only species known to support N2 fixation and functionalization were based on a handful of metals of the s and d blocks of the periodic table. Here we present one-pot binding, cleavage and reduction of N2 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.



中文翻译:

一锅,室温下将二氮转化为主族元素的氯化铵。

将二氮 (N 2 )工业还原为氨是一个能源密集型过程,消耗了全球能源供应的很大一部分。因此,几十年来一直在寻找能够在温和条件下结合 N 2并切割其强 N-N 键的物种。直到最近,已知支持 N 2固定和功能化的唯一物种是基于元素周期表中sd区的少数金属。在这里,我们展示了 N 2的一锅结合、裂解和还原由主族物种转化为铵。该反应——一个复杂的多重还原-质子化序列——在室温下通过使用固相还原剂和酸试剂在单个合成步骤中进行。混合物的简单酸猝灭然后提供铵,存在于肥料中的氨的质子化形式。阐明了该过程中的基本反应步骤,包括关键的 N-N 键断裂过程,并分离了反应的所有中间体。

更新日期:2020-10-19
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