Orjuela Adrián L, Núñez-Zarur Francisco, Alí-Torres Jorge
Departamento de Química, Universidad Nacional de Colombia-Sede Bogotá 111321 Colombia
Facultad de Ciencias Básicas, Universidad de Medellín Carrera 87 No 30-65 050026 Medellín Colombia
RSC Adv. 2022 Sep 7;12(37):24077-24087. doi: 10.1039/d2ra03907a. eCollection 2022 Aug 22.
Iron complexes play a key role in several biological processes, and they are also related to the development of neurological disorders, such as Alzheimer's and Parkinson's diseases. One of the main properties involved in these processes is the standard reduction potential (SRP) of iron complexes. However, the calculation of this property is challenging, mainly due to problems in the electronic structure description, solvent effects and the thermodynamic cycles used for its calculation. In this work, we proposed a computational protocol for the calculation of SRPs of iron complexes by evaluating a wide range of density functionals for the electronic structure description, two implicit solvent models with varying radii and two thermodynamic cycles. Results show that the M06L density functional in combination with the SMD solvation model and the isodesmic method provides good results compared with SRP experimental values for a set of iron complexes. Finally, this protocol was applied to three Fe-Aβ model systems involved in the development of Alzheimer's disease and the obtained SRP values are in good agreement with those reported previously by means of MP2 calculations.
铁配合物在多个生物过程中起着关键作用，并且它们还与神经疾病的发展有关，如阿尔茨海默病和帕金森病。这些过程中涉及的主要性质之一是铁配合物的标准还原电位（SRP）。然而，该性质的计算具有挑战性，主要是由于电子结构描述、溶剂效应以及用于其计算的热力学循环方面存在问题。在这项工作中，我们通过评估用于电子结构描述的多种密度泛函、两种具有不同半径的隐式溶剂模型和两种热力学循环，提出了一种计算铁配合物SRP的计算方案。结果表明，与一组铁配合物的SRP实验值相比，M06L密度泛函与SMD溶剂化模型和等键方法相结合能提供良好的结果。最后，该方案应用于参与阿尔茨海默病发展的三个Fe-Aβ模型系统，所得SRP值与先前通过MP2计算报道的值高度一致。
