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Water Vapor Adsorption on Goethite

机译：针铁矿上水蒸气的吸附

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摘要

Goethite (α-FeOOH) is an important mineral contributing to processes of atmospheric and terrestrial importance. Their interactions with water vapor are particularly relevant in these contexts. In this work, molecular details of water vapor (0.0-19.0 Torr; 0-96% relative humidity at 25 ℃) adsorption at surfaces of synthetic goethite nanoparticles reacted with and without HCl and NaCl were resolved using vibrational spectroscopy. This technique probed interactions between surface (hydr)oxo groups and liquid water-like films. Molecular dynamics showed that structures and orientations adopted by these waters are comparable to those adopted at the interface with liquid water. Particle surfaces reacted with HCl accumulated less water than acid-free surfaces due to disruptions in hydrogen bond networks by chemisorbed waters and chloride. Particles reacted with NaCl had lower loadings below ~10 Torr water vapor but greater loadings above this value than salt-free surfaces. Water adsorption reactions were here affected by competitive hydration of coexisting salt-free surface regions, adsorbed chloride and sodium, as well as precipitated NaCl. Collectively, the findings presented in this study add further insight into the initial mechanisms of thin water film formation at goethite surfaces subjected to variations in water vapor pressure that are relevant to natural systems.
机译：针铁矿（α-FeO​​OH）是重要的矿物，对大气和陆地具有重要意义。在这些情况下，它们与水蒸气的相互作用特别重要。在这项工作中，使用振动光谱法分析了在有或没有HCl和NaCl反应的合成针铁矿纳米颗粒表面吸附的水蒸气（0.0-19.0 Torr； 25℃下相对湿度为0-96％）的分子细节。这项技术探讨了表面（羟基）氧代基与液态水状薄膜之间的相互作用。分子动力学表明，这些水所采用的结构和取向与与液态水的界面处所采用的结构和取向相当。与HCl反应的颗粒表面比无酸表面积累的水少，这是由于化学吸附的水和氯化物破坏了氢键网络。与NaCl反应的颗粒在低于〜10 Torr水蒸气的情况下具有较低的载荷，但在高于该值时，其载荷比无盐表面更大。在此，水吸附反应受到共存的无盐表面区域，吸附的氯化物和钠以及沉淀的NaCl竞争性水合的影响。总的来说，本研究中提出的发现进一步加深了对针铁矿表面水膜形成过程中水膜压力变化的初步机理的初步认识，而水蒸气压力变化与自然系统有关。

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  • 来源
    《Environmental Science & Technology》 |2013年第13期|7171-7177|共7页
  • 作者

    Xiaowei Song; Jean-Francois Boily;

  • 作者单位

    Department of Chemistry, Umea University, SE-901 87 Umea, Sweden;

    Department of Chemistry, Umea University, SE-901 87 Umea, Sweden;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
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