Proton Dynamics at the Water–Silica Interface via Dissociative Molecular Dynamics
Proton Dynamics at the Water–Silica Interface via Dissociative Molecular Dynamics
复制标题
通过解离分子动力学研究水-二氧化硅界面的质子动力学
DOI：
10.1021/jp507640y
复制
发表时间：
2014
影响因子：
3.7
通讯作者：
S. Garofalini
中科院分区：
文献类型：
--
作者：
Glenn K. Lockwood;S. Garofalini
一个强大而准确的解离势，再现了大块和纳米密闭水的结构和动态特性，以及类似于大块水中从头算计算的质子输运，用于二氧化硅/水界面上质子动力学的反应性分子动力学模拟。模拟计算了不同水密度条件下，水与平面非晶态二氧化硅表面和非晶态二氧化硅圆柱孔界面处质子化位点的寿命。除了寿命外，还根据局部原子结构对供体/受体位点进行了评估和讨论。考虑了质子化位点（包括h30 +， SiOH， SiOH2+和Si - (OH+) - Si位点）的寿命结果。水合氢离子h30 +的寿命在界面附近比在散装水中短得多，其他质子化位点的寿命也是如此。结果表明，无定形二氧化硅表面在高温下具有良好的效果。
A robust and accurate dissociative potential that reproduces the structural and dynamic properties of bulk and nanoconfined water, and proton transport similar to ab initio calculations in bulk water, is used for reactive molecular dynamics simulations of the proton dynamics at the silica/water interface. The simulations are used to evaluate the lifetimes of protonated sites at the interfaces of water with planar amorphous silica surfaces and cylindrical pores in amorphous silica with different densities of water confined in the pores. In addition to lifetimes, the donor/acceptor sites are evaluated and discussed in terms of local atomistic structure. The results of the lifetimes of the protonated sites, including H3O+, SiOH, SiOH2+, and Si–(OH+)–Si sites, are considered. The lifetime of the hydronium ion, H3O+, is considerably shorter near the interface than in bulk water, as are the lifetimes of the other protonated sites. The results indicate the beneficial effect of the amorphous silica surface in enh...