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Adsorption of Hydrogen Gas and Redox Processes in Clays

机译:粘土中氢气的吸附和氧化还原过程

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摘要

In order to assess the adsorption properties of hydrogen gas and reactivity of adsorbed hydrogen, we measured H_2(g) adsorption on Na synthetic montmorillonite-type clays and Callovo-Oxfordian (COx) dayrock using gas chromatography. Synthetic montmoriilonites with increasing structural Fe(Ⅲ) substitution (0 wt %, 3.2 wt %, and 6.4 wt % Fe) were used Fe in the synthetic montmoriilonites is principally present as structural Fe(Ⅲ) ions. We studied the concomitant reduction of structural Fe(Ⅲ) in the clays using ~(57)Fe Mossbauer spectrometry. The CO_x, which mainly contains smectite/illite and calcite minerals, is also studied together with the pure clay fraction of this dayrock. Experiments were performed with dry clay samples which were reacted with hydrogen gas at 90 and 120 ℃ for 30 to 45 days at a hydrogen partial pressure close to 0.45 bar. Results indicate that up to 0.11 wt % of hydrogen is adsorbed on the clays at 90 ℃ under 0.45 bar of relative pressure. Fe Mossbauer spectrometry shows that up to 696 of the total structural Fe(Ⅲ) initially present in these synthetic days is reduced upon adsorption of hydrogen gas. No reduction is observed with the CO_x sample in the present experimental conditions.
机译:为了评估氢气的吸附性能和吸附的氢气的反应性,我们使用气相色谱法测量了Na合成蒙脱土型粘土和Callovo-Oxfordian(COx)日岩上的H_2(g)吸附。使用具有增加的结构Fe(Ⅲ)取代度(0 wt%,3.2 wt%和6.4 wt%Fe)的合成蒙脱土,合成蒙脱土中的Fe主要以结构Fe(Ⅲ)离子的形式存在。我们用〜(57)Fe Mossbauer光谱研究了粘土中结构性Fe(Ⅲ)的伴随还原。还研究了主要含有绿土/伊利石和方解石矿物的CO_x以及该日岩的纯粘土成分。用干燥的粘土样品进行实验,该样品在氢气分压接近0.45 bar的条件下与氢气在90和120℃下反应30至45天。结果表明,在90℃,0.45 bar的相对压力下,最多有0.11 wt%的氢吸附在粘土上。 Fe Mossbauer光谱法显示,在这些合成天中最初存在的全部结构Fe(Ⅲ)中,多达696种在吸附氢气后被还原。在目前的实验条件下,CO_x样品未见减少。

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  • 来源
    《Environmental Science & Technology》 |2012年第6期|p.3574-3579|共6页
  • 作者单位

    ISTerre, Environmental Geochemistry Group, Observatory for Earth and Planetary Sciences, Grenoble University, 38041 Grenoble Cedex 9, France,ANDRA, National Radioactive Waste Management Agency, Science Department, 92298 Chatenay-Malabry Cedex, France,CEA/LITEN/DTNM/LCSN, Laboratory of Chemistry and Nanomaterials Safety, 38054 Grenoble Cedex, France;

    ISTerre, Environmental Geochemistry Group, Observatory for Earth and Planetary Sciences, Grenoble University, 38041 Grenoble Cedex 9, France,ANDRA, National Radioactive Waste Management Agency, Science Department, 92298 Chatenay-Malabry Cedex, France;

    LUNAM Universite du Maine, Institut des Molecules et Materiaux du Mans, UMR CNRS 6283, 72085 Le Mans Cedex, France;

    ANDRA, National Radioactive Waste Management Agency, Science Department, 92298 Chatenay-Malabry Cedex, France;

    ISTerre, Environmental Geochemistry Group, Observatory for Earth and Planetary Sciences, Grenoble University, 38041 Grenoble Cedex 9, France;

  • 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);
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  • 正文语种 eng
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