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Examination of Protonation-Induced Dinitrogen Splitting by in Situ EXAFS Spectroscopy.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-09-22 , DOI: 10.1021/acs.inorgchem.0c02134 Josh Abbenseth 1 , Jean-Pierre H Oudsen 2 , Bas Venderbosch 2 , Serhiy Demeshko 1 , Markus Finger 1 , Christian Herwig 3 , Christian Würtele 1 , Max C Holthausen 4 , Christian Limberg 3 , Moniek Tromp 5 , Sven Schneider 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-09-22 , DOI: 10.1021/acs.inorgchem.0c02134 Josh Abbenseth 1 , Jean-Pierre H Oudsen 2 , Bas Venderbosch 2 , Serhiy Demeshko 1 , Markus Finger 1 , Christian Herwig 3 , Christian Würtele 1 , Max C Holthausen 4 , Christian Limberg 3 , Moniek Tromp 5 , Sven Schneider 1
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The splitting of dinitrogen into nitride complexes emerged as a key reaction for nitrogen fixation strategies at ambient conditions. However, the impact of auxiliary ligands or accessible spin states on the thermodynamics and kinetics of N–N cleavage is yet to be examined in detail. We recently reported N–N bond splitting of a {Mo(μ2:η1:η1-N2)Mo}-complex upon protonation of the diphosphinoamide auxiliary ligands. The reactivity was associated with a low-spin to high-spin transition that was induced by the protonation reaction in the coordination periphery, mainly based on computational results. Here, this proposal is evaluated by an XAS study of a series of linearly N2 bridged Mo pincer complexes. Structural characterization of the transient protonation product by EXAFS spectroscopy confirms the proposed spin transition prior to N–N bond cleavage.
中文翻译：
通过原位EXAFS光谱检查质子化诱导的二氮分裂。
在环境条件下，将氮分解为氮化物络合物是固氮策略的关键反应。但是，辅助配体或可接近的自旋态对N–N裂解的热力学和动力学的影响尚待详细研究。我们最近报道了的N-N键断裂{沫（μ 2：η 1：η 1 -N 2）莫} -配合物在所述diphosphinoamide辅助配体的质子化。主要基于计算结果，反应性与配位周围质子化反应诱导的从低旋向高旋的转变有关。在这里，通过XAS研究一系列线性N 2来评估该建议桥接的Mo钳配合物。通过EXAFS光谱对瞬态质子化产物的结构表征证实了在N–N键断裂之前提议的自旋转变。
更新日期：2020-10-05
中文翻译：
通过原位EXAFS光谱检查质子化诱导的二氮分裂。
在环境条件下，将氮分解为氮化物络合物是固氮策略的关键反应。但是，辅助配体或可接近的自旋态对N–N裂解的热力学和动力学的影响尚待详细研究。我们最近报道了的N-N键断裂{沫（μ 2：η 1：η 1 -N 2）莫} -配合物在所述diphosphinoamide辅助配体的质子化。主要基于计算结果，反应性与配位周围质子化反应诱导的从低旋向高旋的转变有关。在这里，通过XAS研究一系列线性N 2来评估该建议桥接的Mo钳配合物。通过EXAFS光谱对瞬态质子化产物的结构表征证实了在N–N键断裂之前提议的自旋转变。
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