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首页> 外文期刊>The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical >First Computational Evidence of a Competitive Stepwise and Concerted Mechanism for the Reduction of Antimalarial Endoperoxides
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First Computational Evidence of a Competitive Stepwise and Concerted Mechanism for the Reduction of Antimalarial Endoperoxides

机译：竞争性逐步协调一致的机制减少疟疾内过氧化物的第一个计算证据

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摘要

We study structural analogues of endoperoxides belonging to the family of G factors which present moderate to good antimalarial activity. Their biological activity is related to the reduction and cleavage of the O-O bond. Generally, the O-O bond reduction of model endoperoxides, as well as artemisinin, occurs by a concerted dissociative electron transfer (ET) mechanism. For the G3 and G3Me compounds, the experimental counterpart indicates an unexpected competition between a concerted and a stepwise mechanism, but no intermediate species can be isolated. We thus perform DFT studies on the reduction of G3 and G3Me compounds. We confirm the formation of an intermediate radical anion followed by cleavage of the O-O bond in a second step. We characterize the stable conformations for the radical anions G3~(·-) and G3Me~(·-) resulting from the ET and the associated reaction pathway. We also calculate the reorganization energy upon ET in relation to the Marcus theory using the DFT method. These results provide valuable insight into understanding the biological activity of G-factor endoperoxides as potential therapeutic antimalarial agents.
机译：我们研究属于G因子家族的内过氧化物的结构类似物，其表现出中等至良好的抗疟活性。它们的生物活性与O-O键的还原和裂解有关。通常，模型内过氧化物以及青蒿素的O-O键还原是通过协同的解离电子转移（ET）机制发生的。对于G3和G3Me化合物，实验对象表明协同机制和逐步机制之间存在意想不到的竞争，但无法分离出任何中间物种。因此，我们对D3和G3Me化合物的还原进行了DFT研究。我们确认形成了中间自由基阴离子，然后在第二步中裂解了O-O键。我们表征了由ET及其相关的反应途径产生的自由基阴离子G3〜（·-）和G3Me〜（·-）的稳定构象。我们还使用DFT方法相对于Marcus理论计算了ET的重组能量。这些结果为了解G因子过氧化物作为潜在治疗性抗疟药的生物学活性提供了宝贵的见识。

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