Low-Coordinate Iron Hydride Chemistry at an N,N,C-Heteroscorpionate Platform,Inorganic Chemistry

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Low-Coordinate Iron Hydride Chemistry at an N,N,C-Heteroscorpionate Platform
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2024-07-22 , DOI: 10.1021/acs.inorgchem.4c01596
Addison Fraker ₁ , Brittany N Linn ₂ , Alex McSkimming ₁

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Locally high-spin iron hydrides are proposed to play a critical role as intermediates in iron–molybdenum cofactor (FeMoco)-catalyzed N₂ fixation. Inspired by these biological systems, we report herein our initial investigations into low-coordinate iron hydride chemistry supported by our N,N,C-heteroscorpionate ligands. Those ligands with smaller steric profiles are unable to completely suppress the formation of a binuclear [Fe(μ₂-H)]₂ complex; however, the incorporation of more substantial steric bulk allows for the isolation of a rare example of a terminal, high-spin (S = 2) Fe²⁺ hydride. Fourier transform infrared spectroscopy suggests an unusually weak Fe–H bond in the latter molecule. Mössbauer spectroscopies, coupled with density functional theory calculations, highlights the substantial influence of the terminal hydride ligand on ⁵⁷Fe isomer shift.

中文翻译：

N,N,C-杂蝎酸酯平台上的低配位氢化铁化学

局部高自旋铁氢化物被认为作为铁钼辅助因子（FeMoco）催化的 N ₂固定中的中间体发挥着关键作用。受这些生物系统的启发，我们在此报告了我们对 N,N,C-杂蝎酸配体支持的低配位氢化铁化学的初步研究。那些具有较小空间分布的配体不能完全抑制双核[Fe(μ ₂ -H)] ₂配合物的形成；然而，结合更多的空间体积可以分离出罕见的末端高自旋 ( S = 2) Fe ²⁺氢化物。傅里叶变换红外光谱表明后一个分子中存在异常弱的 Fe-H 键。穆斯堡尔谱与密度泛函理论计算相结合，强调了末端氢化物配体对⁵⁷ Fe 异构体位移的重大影响。

更新日期：2024-07-22

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