Catalytically Active Iron(IV)oxo Species Based on a Bis(pyridinyl)phenanthrolinylmethane,Israel Journal of Chemistry

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Catalytically Active Iron(IV)oxo Species Based on a Bis(pyridinyl)phenanthrolinylmethane
Israel Journal of Chemistry ( IF 2.3 ) Pub Date : 2020-03-30 , DOI: 10.1002/ijch.202000009
Henrika M. Hüppe ₁ , Kristina Keisers ₁ , Fabian Fink ₁ , Sonja D. Mürtz ₁ , Alexander Hoffmann ₁ , Linda Iffland ₂ , Ulf-Peter Apfel _{2,

3} , Sonja Herres-Pawlis ₁

Affiliation

Starting from the mononuclear iron(II) complex [Fe(MeCPy₂Phen)(MeCN)₂]²⁺, a non‐heme Fe(IV)oxo complex [Fe^IV(MeCPy₂Phen)O]²⁺ was synthesized via oxidation with meta‐chloroperoxybenzoic acid (mCPBA). The Fe(IV)oxo complex was characterized using UV/Vis spectroscopy, Mößbauer spectroscopy and CSI mass spectrometry. The ability of this species to oxidize C−H bonds was tested with cyclohexane and adamantane as model substrates. For cyclohexane, an alcohol‐to‐ketone ratio (A/K) of 6.1 and efficiencies up to 55 were obtained. In case of adamantane, the ratio of tertiary over secondary products (3°/2°) is 38. In combination, this indicates the iron(IV)oxo complex being the catalytically active species.

中文翻译：

基于双（吡啶基）菲咯啉基甲烷的催化活性铁（IV）氧物种

从单核铁（II）配合物[Fe（MeCPy ₂ Phen）（MeCN）₂ ] ²⁺出发，通过氧化合成非血红素Fe（IV）氧配合物[Fe ^IV（MeCPy ₂ Phen）O] ²⁺与间-氯过氧苯甲酸（mCPBA）。使用紫外/可见光谱，穆斯堡尔光谱和CSI质谱仪对Fe（IV）羰基配合物进行了表征。以环己烷和金刚烷为模型底物，测试了该物种氧化CH键的能力。对于环己烷，醇与酮之比（A / K）的6.1，效率高达55。在金刚烷的情况下，第三级产物与次级产物的比率（3°/ 2°）为38。综合而言，这表明铁（IV）氧杂络合物是催化活性物质。

更新日期：2020-03-30

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