Polarizable and Non-Polarizable Force Field Representations of Ferric Cation and Validations
Polarizable and Non-Polarizable Force Field Representations of Ferric Cation and Validations
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三价铁阳离子的极化和非极化力场表示及验证
DOI：
10.1021/acs.jpcb.7b02010
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发表时间：
2017
影响因子：
3.3
通讯作者：
Wang Dongqi
中科院分区：
文献类型：
--
作者：
Xia Miaoren;Chai Zhifang;Wang Dongqi
对铁离子的阿米巴极化力场进行了优化，并将其应用于研究铁离子在水相中的水化及其与卟啉的络合。为便于比较，对不可极化力场也进行了优化。相对于实验数据，阿米巴力场给出了比不可极化力场更准确的水化自由能，并正确地预测了水合Fe3+的最稳定电子态(六重态)和Fe(III)-POR络合物的最稳定电子态(四重态)，这与用密度泛函方法进行的文献一致。为了得到极化能和范德华能的精确图像，显式包含Fe3+和配体之间的电荷转移是很重要的，否则就会偏离从头计算得到的相应的能量分量。阿米巴力场在表征水-Fe(III)-POR络合物中的成功应用表明，通过可靠地处理金属原子与蛋白质之间的相互作用，该力场可以扩展到研究含高电荷金属离子的金属酶在凝聚相中的动力学。
The AMOEBA polarizable force field of ferric ion was optimized and applied to study the hydration of ferric ion and its complexation with porphine in the aqueous phase. The nonpolarizable force field was also optimized for comparison. The AMOEBA force field was found to give a more accurate hydration free energy than the nonpolarizable force field with respect to experimental data, and correctly predict the most stable electronic state of hydrated Fe3+, which is the sextet state, and of the Fe(III)–Por complex, which is the quartet state, consistent with the literature that was carried out using the DFT method. The explicit inclusion of charge transfer between Fe3+and ligand was found to be important in order to obtain a precise picture of polarization energy and van der Waals energy, which otherwise deviate from the corresponding energy components derived from ab initio calculations. The successful application of the AMOEBA force field in the characterization of aquo Fe(III)–Por complexes suggests that its use may be extended to the study of the dynamics of metalloenzyme containing highly charged metal ions in the condensed phase with reliable treatment of the interactions between metal atom and protein.