Physical Sciences Division, Pacific Northwest National Laboratory, MSIN K8-88, P.O. Box 999, Richland, WA 99352, USA.
Phys Chem Chem Phys. 2018 May 3;20(17):11634-11642. doi: 10.1039/c8cp01284a.
The radiation-induced decomposition and desorption of nanoscale amorphous solid water (D2O) films adsorbed on an α-Al2O3(0001) surface was studied at low temperature in ultrahigh vacuum using temperature programmed desorption (TPD) and electron stimulated desorption (ESD) with a mono-energetic, low energy electron source. ESD yields of molecular products (D2, O2 and D2O) and the total sputtering yield increased with increasing D2O coverage up to ∼15 water monolayers (i.e. ∼15 × 1015 cm-2) to a coverage-independent level for thicker water films. Experiments with isotopically-layered water films (D2O and H2O) demonstrated that the highest water decomposition yields occurred at the interfaces of the nanoscale water films with the alumina substrate and vacuum. However, the increased reactivity of the water/alumina interface is relatively small compared to the enhancements in the non-thermal reactions previously observed at the water/Pt(111) and water/TiO2(110) interfaces. We propose that the relatively low activity of Al2O3(0001) for the radiation-induced production of molecular hydrogen is associated with lower reactivity of this surface with hydrogen atoms, which are likely precursors for the formation of molecular hydrogen.
在超高真空中,使用具有单能量、低能电子源的程序升温脱附(TPD)和电子刺激脱附(ESD)技术,研究了吸附在α-Al2O3(0001)表面上的纳米级非晶态水(D2O)薄膜在低温下的辐射诱导分解和解吸。随着 D2O 覆盖度的增加(最高可达约 15 个水单层,即约 15×1015cm-2),分子产物(D2、O2 和 D2O)的 ESD 产率和总溅射产率增加到一个与水膜厚度无关的水平。对于具有同位素层的水膜(D2O 和 H2O)的实验表明,在纳米级水膜与氧化铝基底和真空的界面处,水的分解产率最高。然而,与先前在水/Pt(111)和水/TiO2(110)界面观察到的非热反应增强相比,水/氧化铝界面的增强相对较小。我们提出,Al2O3(0001)对于辐射诱导产生分子氢的相对低活性与该表面与氢原子的低反应性有关,氢原子可能是分子氢形成的前体。