Mechanochemistry at Solid Surfaces: Polymerization of Adsorbed Molecules by Mechanical Shear at Tribological Interfaces
Mechanochemistry at Solid Surfaces: Polymerization of Adsorbed Molecules by Mechanical Shear at Tribological Interfaces
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DOI：
10.1021/acsami.6b14159
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发表时间：
2017-01-25
影响因子：
9.5
通讯作者：
Kim, Seong H.
中科院分区：
文献类型：
--
作者：
Yeon, Jejoon;He, Xin;Kim, Seong H.
采用气相润滑条件下的摩擦试验和反应分子动力学模拟研究了烯丙醇在氧化硅界面上的吸附和剪切聚合反应。从实验和模拟得到的产物形成的负载依赖性是一致的，表明在模拟中观察到的原子尺度过程与实验相关。在机械辅助热反应理论的背景下，结合从模拟中获得的原子细节的实验结果的分析表明，由机械剪切引起的烯丙醇分子的缔合反应途径是完全不同的化学诱导的聚合反应。研究结果表明，一定程度的扭曲的分子从其平衡状态是必要的机械诱导的化学反应发生和这样的扭曲发生在机械剪切时，分子共价锚定到一个滑动表面。
Polymerization of allyl alcohol adsorbed and sheared at a silicon oxide interface is studied using tribo-tests in vapor phase lubrication conditions and reactive molecular dynamics simulations. The load dependences of product formation obtained from experiments and simulations were consistent, indicating that the atomic-scale processes observable in the simulations were relevant to the experiments. Analysis of the experimental results in the context of mechanically assisted thermal reaction theory, combined with the atomistic details available from the simulations, suggested that the association reaction pathway of allyl alcohol molecules induced by mechanical shear is quite different from chemically induced polymerization reactions. Findings suggested that some degree of distortion of the molecule from its equilibrium state is necessary for mechanically induced chemical reactions to occur and such a distortion occurs during mechanical shear when molecules are covalently anchored to one of the sliding surfaces.