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

近年来，我们已经能够为氧激活的非血红素铁酶的代表，如半胱氨酸双加氧酶(CDO)、2-氨基乙硫醇双加氧酶(ADO)和1-氨基环丙烷-1-羧酸氧化酶(ACCO)开发出相当真实的基于三吡唑基硼酸盐的结构和功能模型。然而，由于其多步转化的复杂性，到目前为止，机械信息只能间接获取，中间体的捕获和实验鉴定到目前为止仍然具有挑战性。该项目的主要目标是通过精心选择和设计的配基体系构建忠实的模型化合物，帮助理解这类单核非血红素铁酶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。重点将特别放在瞬时物种的鉴定上，以揭示这些酶固有的反应原理，作为开发合成氧活化铁催化剂的基础，而For团队内部的合作将是关键。

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.