Influence of imidazole functionalization on the properties of small molecule models of the LPMO active site†

IF 3.3 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Dalton Transactions Pub Date : 2025-03-20 DOI:10.1039/D4DT03424D
Ugo Gilbert, Xiao Mu, Yan Yu Sarah Lam, Gaël De Leener, Martin Schoenauen, Maëlle Bottin, Koen Robeyns, Michel Luhmer, Raphaël Robiette and Michael L. Singleton
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Abstract

A series of small molecule Cu(II) complexes based on tridentate N3 ligands relevant to the histidine brace of the active site of lytic polysaccharide monooxygenase were synthesized and characterized by X-ray crystallography and spectroscopic studies. In order to better understand the role of different structural features and to help bridge the differences between previously reported models, the methylation patterns, imidazole connectivity, linker nature, and type of heterocycle were systematically varied across the series. These modifications lead to important differences in the electrochemical properties of the complexes and their reactivity towards the oxidation of a model substrate.

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咪唑功能化对LPMO活性位点小分子模型性质的影响
合成了一系列基于与多糖单加氧酶活性位点组氨酸支相关的三齿N3配体的小分子Cu(II)配合物,并用x射线晶体学和光谱研究对其进行了表征。为了更好地理解不同结构特征的作用,并帮助弥合先前报道的模型之间的差异,甲基化模式、咪唑连通性、连接物性质和杂环类型在整个系列中系统地变化。这些修饰导致配合物的电化学性质和它们对模型底物氧化的反应性的重要差异。
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来源期刊
Dalton Transactions
Dalton Transactions 化学-无机化学与核化学
CiteScore
6.60
自引率
7.50%
发文量
1832
审稿时长
1.5 months
期刊介绍: Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.
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