Adsorption and Diffusion of Oxygen on Pure and Partially Oxidized Metal Surfaces in Ultrahigh Resolution
Adsorption and Diffusion of Oxygen on Pure and Partially Oxidized Metal Surfaces in Ultrahigh Resolution
复制标题
超高分辨率氧气在纯金属和部分氧化金属表面的吸附和扩散
DOI：
10.1021/acs.nanolett.2c00490
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发表时间：
2022
期刊：
影响因子：
10.8
通讯作者：
Heinz, Hendrik
中科院分区：
文献类型：
--
作者：
Kanhaiya, Krishan;Heinz, Hendrik
气体分子与金属和氧化物表面的相互作用在腐蚀、催化、传感和异质材料中起着关键作用。然而，到目前为止，对O2从皮秒到微秒的动态的了解仍然不可用。我们获得了O2在Ni和Al的11种常见的原始和部分氧化（hkl）表面上吸附的3D势能面，其分辨率为皮米，精度为0.1 kcal/mol，确定了结合位点，并在25至300 °C范围内获得了表面迁移率。我们解释了氧化物生长的相对氧化速率和参数。我们使用来自X射线衍射（XRD）和低能电子衍射（LEED）的结构数据，使用界面力场（IFF）进行了超过15万次分子力学和分子动力学模拟。该方法的准确度比以前高10至50倍，适用于分析气体与金属的相互作用，最高可达微米级，包括缺陷和不规则纳米结构。
The interaction of gas molecules with metal and oxide surfaces plays a critical role in corrosion, catalysis, sensing, and heterogeneous materials. However, insights into the dynamics of O2from picoseconds to microseconds have remained unavailable to date. We obtained 3D potential energy surfaces for adsorption of O2on 11 common pristine and partially oxidized (hkl) surfaces of Ni and Al in picometer resolution and high accuracy of 0.1 kcal/mol, identified binding sites, and surface mobility from 25 to 300 °C. We explain relative oxidation rates and parameters for oxide growth. We employed over 150 000 molecular mechanics and molecular dynamics simulations with the interface force field (IFF) using structural data from X-ray diffraction (XRD) and low-energy electron diffraction (LEED). The methods reach 10 to 50 times higher accuracy than possible before and are suited to analyze gas interactions with metals up to the micrometer scale including defects and irregular nanostructures.