Understanding and advancing the reactivity of biomimetic models for mononuclear non-heme iron enzymes

了解和推进单核非血红素铁酶仿生模型的反应性

• 批准号: 495385999
• 负责人: Professor Dr. Christian Limberg
• 金额: --
• 依托单位: Arbeitsgruppe Koordinationschemie / Katalyse
• 依托单位国家: 德国
• 项目类别: Research Units
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/495385999?language=en
• 关键词: Understanding; advancing; reactivity; biomimetic; models

In recent years we have been able to develop rather realistic trispyrazolyl borate-based structural and functional models for representatives of O2-activating non-heme iron enzymes, like the Cysteine Dioxygenase (CDO), the 2-Aminoethanethiol Dioxygenase (ADO) and the 1-Aminocyclopropane-1-carboxylic acid Oxidase (ACCO). However, due to the complexity of their multi-step conversions mechanistic information until now could only be accessed indirectly, and the trapping and experimental identification of intermediates has so far remained challenging. The main goal of this project is to contribute to the understanding of the complicated mechanisms, by which such mononuclear non-heme iron enzymes convert their amino acid substrates and the cysteine-related aminoethanethiol, respectively, with the aid of faithful model compounds constructed with carefully selected and designed ligand systems. Particular emphasis will lie on the identification of transient species to reveal the reaction principles inherent to such enzymes as a basis for the development of synthetic O2-activating iron catalysts, and cooperations within the FOR team will be key.

近年来，我们已经能够开发出相当现实的三吡唑硼酸酯为基础的结构和功能模型的代表O2-激活非血红素铁酶，如半胱氨酸双加氧酶（CDO），2-氨基乙烷乙氧基双加氧酶（ADO）和1-氨基环丙烷-1-羧酸氧化酶（ACCO）。然而，由于其多步转化的复杂性，迄今为止只能间接获得机械信息，并且中间体的捕获和实验鉴定迄今为止仍然具有挑战性。该项目的主要目标是帮助理解这种单核非血红素铁酶在精心选择和设计的模型化合物的帮助下分别转化其氨基酸底物和半胱氨酸相关的氨基乙硫醇的复杂机制。配体系统。 特别强调将在于识别的瞬态物种，以揭示这种酶作为合成O2活化铁催化剂的发展的基础上固有的反应原理，并在FOR团队的合作将是关键。