首页> 外文期刊>The Journal of Chemical Physics >Oxygen diffusion and reactivity at low temperature on bare amorphous olivine-type silicate
【24h】

Oxygen diffusion and reactivity at low temperature on bare amorphous olivine-type silicate

机译:裸露无定形橄榄石型硅酸盐在低温下的氧扩散和反应性

获取原文
获取原文并翻译 | 示例
           

摘要

The mobility of O atoms at very low temperatures is not generally taken into account, despite O diffusion would add to a series of processes leading to the observed rich molecular diversity in space. We present a study of the mobility and reactivity of O atoms on an amorphous silicate surface. Our results are in the form of reflection absorption infrared spectroscopy and temperature-programmed desorption spectra of O_2 and O_3 produced via two pathways: O + O and O_2 + O, investigated in a submonolayer regime and in the range of temperature between 6.5 and 30 K. All the experiments show that ozone is formed efficiently on silicate at any surface temperature between 6.5 and 30 K. The derived upper limit for the activation barriers of O + O and O_2 + O reactions is ~150 K/k_b. Ozone formation at low temperatures indicates that fast diffusion of O atoms is at play even at 6.5 K. Through a series of rate equations included in our model, we also address the reaction mechanisms and show that neither the Eley-Rideal nor the hot atom mechanisms alone can explain the experimental values. The rate of diffusion of O atoms, based on modeling results, is much higher than the one generally expected, and the diffusive process proceeds via the Langmuir-Hinshelwood mechanism enhanced by tunnelling. In fact, quantum effects turn out to be a key factor that cannot be neglected in our simulations. Astrophysically, efficient O_3 formation on interstellar dust grains would imply the presence of huge reservoirs of oxygen atoms. Since O_3 is a reservoir of elementary oxygen, and also of OH via its hydrogenation, it could explain the observed concomitance of CO_2 and H_2O in the ices.
机译:尽管O扩散会增加一系列过程,导致观察到的丰富的空间分子多样性,但通常不会考虑O原子在非常低的温度下的迁移率。我们目前对非晶硅酸盐表面上O原子的迁移率和反应性的研究。我们的结果采用反射吸收红外光谱的形式以及通过以下两种途径产生的O_2和O_3的程序升温脱附光谱:O + O和O_2 + O,在亚单层体系中以及在6.5至30 K的温度范围内进行了研究。所有实验表明,在6.5至30 K的任何表面温度下,臭氧都能在硅酸盐上有效地形成,得出的O + O和O_2 + O反应活化能的上限为〜150 K / k_b。低温下的臭氧形成表明,即使在6.5 K时,O原子的快速扩散也起作用。通过我们模型中包含的一系列速率方程,我们还讨论了反应机理,并没有发现Eley-Rideal或热原子机理单独可以解释实验值。根据建模结果,O原子的扩散速率比通常预期的要高得多,扩散过程是通过隧道效应增强的Langmuir-Hinshelwood机理进行的。实际上,量子效应被证明是在我们的仿真中不能忽略的关键因素。从天体上看,在星际尘埃颗粒上有效形成O_3意味​​着存在巨大的氧原子储集层。由于O_3是元素氧以及通过其氢化而生成的OH的储存库,因此可以解释在冰中观察到的CO_2和H_2O的混合体。

著录项

相似文献

  • 外文文献
  • 中文文献
  • 专利
获取原文

客服邮箱:kefu@zhangqiaokeyan.com

京公网安备:11010802029741号 ICP备案号:京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有
  • 客服微信

  • 服务号