Development and validation of a ReaxFF reactive force field for Cu cation/water interactions and copper metal/metal oxide/metal hydroxide condensed phases.
Development and validation of a ReaxFF reactive force field for Cu cation/water interactions and copper metal/metal oxide/metal hydroxide condensed phases.
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DOI：
10.1021/jp102272z
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发表时间：
2010-09-09
影响因子：
2.9
通讯作者：
Hermansson, Kersti
中科院分区：
文献类型：
--
作者：
van Duin, Adri C. T.;Bryantsev, Vyacheslav S.;Diallo, Mamadou S.;Goddard, William A.;Rahaman, Obaidur;Doren, Douglas J.;Raymand, David;Hermansson, Kersti
为了使大规模的氧化铜/水和铜离子/水的相互作用的反应动力学模拟，我们已经扩展了ReaxFF反应力场框架的Cu/O/H相互作用。为此，我们采用了多级力场开发策略，其中初始训练集（包含金属/金属氧化物/金属氢氧化物凝聚相数据和[Cu（H2O）n]2+-簇结构和能量）通过从ReaxFF分子动力学模拟中提取的[Cu（H2O）n]2+-簇的单点QM-能量来增强。这为丰富训练集和验证最终力场提供了一种方便的策略。为了进一步验证力场的描述，我们进行了分子动力学模拟的Cu 2 +/水系统。我们发现我们的结果和早期的实验和基于量子力学的分子动力学工作之间的平均Cu/水的协调，Jahn-Teller扭曲和反转[Cu（H2O）6]2+-集群，第一和第二壳层O-Cu-O的角分布，表明该力场给出了一个令人满意的描述的Cu-阳离子/水的相互作用。我们相信，这个力场提供了一个计算方便的方法，用于研究溶液和表面化学的金属阳离子和金属氧化物，因此，有研究蛋白质/金属阳离子复合物，pH值依赖的晶体生长/溶解和表面催化的应用。
In order to enable large-scale reactive dynamic simulations of copper oxide/water and copper ion/water interactions we have extended the ReaxFF reactive force field framework to Cu/O/H interactions. To this end, we employed a multistage force field development strategy, where the initial training set (containing metal/metal oxide/metal hydroxide condensed phase data and [Cu(H2O)n]2+-cluster structures and energies) is augmented by single-point QM-energies from [Cu(H2O)n]2+-clusters abstracted from a ReaxFF molecular dynamics simulation. This provides a convenient strategy to both enrich the training set and to validate the final force field. To further validate the force field description we performed molecular dynamics simulations on Cu2+/water systems. We found good agreement between our results and earlier experimental and QM-based molecular dynamics work for the average Cu/water coordination, Jahn-Teller distortion and inversion in [Cu(H2O)6]2+-clusters, and first- and second shell O-Cu-O angular distributions, indicating that this force field gives a satisfactory description of the Cu-cation/water interactions. We believe that this force field provides a computationally convenient method for studying the solution and surface chemistry of metal cations and metal oxides and, as such, has applications for studying protein/metal cation complexes, pH-dependent crystal growth/dissolution and surface catalysis.
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