Nitrogen Oxyanion Reductive Borylation at Low-Coordinate Iron: A Struggle between Two Oxophiles.

IF 4.3 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Bao G Tran, Nobuyuki Yamamoto, Maren Pink, Yaroslav Losovyj, Kenneth G Caulton, Jeremy M Smith
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引用次数: 0

Abstract

With the advent of the Haber-Bosch process over a century ago, the world's population experienced tremendous growth due to the million tons of fixed nitrogen used in fertilizer each year. However, the majority of the fixed nitrogen is metabolized to various nitrogen oxyanions by soil organisms that are lost to waterways, leading to eutrophication and hypoxia. Therefore, there is a need to convert the anthropogenic nitrogen content to more useful forms. In this work, the synthesis and characterization of iron nitrate (PhB(iPr2Im)3FeNO3) complex (2) is reported. Subsequent stepwise deoxygenation via a bis(boryl) reduced N-heterocycle (BPin2pz) to its downstream counterparts is thermodynamically favorable by DFT. Reaction of iron nitrate with (BPin2)pz led to the formation of iron (pinacolato)boralanolate complex (3) and a proposed diiron dinitrosyl complex having bridged hydroxide ligands ([PhB(iPr2Im)3Fe(NO)(OH)]2) (4). The formation of these complexes demonstrates the oxophilicity of both iron and boron.

低配位铁上的氮氧阴离子还原硼化:两种亲氧试剂之间的斗争。
随着一个多世纪前哈伯-博世法的出现,世界人口经历了巨大的增长,因为每年有数百万吨的固定氮被用于肥料。然而,大部分固定氮被土壤生物代谢为各种氮氧离子,这些氮氧离子流失到水道中,导致富营养化和缺氧。因此,有必要将人为氮含量转化为更有用的形式。本文报道了硝酸铁(PhB(iPr2Im)3FeNO3)配合物(2)的合成和表征。随后通过双(硼基)还原的n -杂环(BPin2pz)逐步脱氧到其下游对应物在热力学上是有利的。硝酸铁与(BPin2)pz反应生成(pinacolato)硼酸铁配合物(3)和二铁二硝基配合物([PhB(iPr2Im)3Fe(NO)(OH)]2)(4)。这些配合物的形成证明了铁和硼的亲氧性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
期刊介绍: Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.
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