Santos José L F, Kauffmann Angélica C, da Silva Sebastião C, Silva Virgínia C P, de Souza Gabriel L C
Departamento de Química, Universidade Federal de Mato Grosso, Cuiabá, Mato Grosso, 78060-900, Brazil.
Department of Chemistry, Washington State University, Pullman, WA, 99164, USA.
J Mol Model. 2020 Aug 17;26(9):233. doi: 10.1007/s00894-020-04469-3.
In this work, we present a computational investigation on the structure and energetics of eleocarpanthraquinone, a newly isolated polyphenolic anthrone-antraquinone. Properties such as bond lengths, angles, atomic charges, bond dissociation enthalpies (BDEs), and ionization potential (IP) were determined through the use of density functional theory (DFT). The B3LYP and M06-2X exchange-correlation functionals were employed along with the 6-31+G(d,p), 6-31+ +G(d,p), and 6-311+G(d,p) basis sets for performing computations in the gas-phase, water, methanol, and ethanol. The conformation presenting all the hydroxyl groups undergoing hydrogen-bond interactions with neighboring oxygen atoms (conformation 5) was assigned as the most stable structure while its counterpart presenting no hydrogen-bond interaction was found to be 36.45 kcal/mol less stable than conformation 5 in the potential energy surface probed at the B3LYP/6-311+G(d,p) level of theory in the gas-phase, for instance. More importantly, the lowest O-H bond dissociation enthalpy was determined to be 93.80 kcal/mol at the B3LYP/6-311+G(d,p) level of theory in water against the 146.58 kcal/mol regarding the IP computed at the same approach, suggesting the hydrogen atom transfer mechanism as being preferred over the single electron transfer mechanism in regards to the antioxidant potential for the case of eleocarpanthraquinone; the same conclusion was drawn from the outcomes of all the other approaches used.
在这项工作中,我们对新分离出的多酚蒽酮 - 蒽醌类化合物eleocarpanthraquinone的结构和能量学进行了计算研究。通过使用密度泛函理论(DFT)确定了诸如键长、键角、原子电荷、键解离焓(BDEs)和电离势(IP)等性质。采用B3LYP和M06 - 2X交换相关泛函以及6 - 31 + G(d,p)、6 - 31 + +G(d,p)和6 - 311 + G(d,p)基组,在气相、水、甲醇和乙醇中进行计算。所有羟基都与相邻氧原子发生氢键相互作用的构象(构象5)被确定为最稳定的结构,而在气相中,在B3LYP/6 - 311 + G(d,p)理论水平探测的势能面上,其不存在氢键相互作用的对应构象比构象5的稳定性低36.45千卡/摩尔。例如,更重要的是,在水中,B3LYP/6 - 311 + G(d,p)理论水平下确定的最低O - H键解离焓为93.80千卡/摩尔,而采用相同方法计算的IP为146.58千卡/摩尔,这表明就eleocarpanthraquinone的抗氧化潜力而言,氢原子转移机制比单电子转移机制更受青睐;从所有其他使用的方法的结果中也得出了相同的结论。