厌氧条件下生物岩在 pH 值为 4 和 6.5 时的溶解动力学以及溶解铁(II)的释放

IF 3.6 2区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Chemical Geology Pub Date : 2024-06-05 DOI:10.1016/j.chemgeo.2024.122204
Stellan Holgersson , Henrik Drake , Andreas Karlsson , Lindsay Krall
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引用次数: 0

摘要

生物岩是花岗岩基岩中主要的含铁矿物,它的溶解对氧气进入后还原条件的修复具有特别重要的意义,例如在采矿活动或建造有毒废物深层储存库之后。本研究调查了在室温、pH 值为 4 和 6.5 的厌氧条件下,对粒度为 0.053-0.075 毫米的生物岩进行最长达 160 天的沥滤。监测了沥滤溶液中主要元素浓度的变化。与 pH 值无关的速率系数 kH+ 分别为 4.8∙10-10、6.9∙10-10、6.3∙10-11 和 1.0∙10-12 mol1-n m-2 s-1。相应的质子反应阶数 nH+ 分别为 0.61、0.63、0.33 和 0.09。由于怀疑在 pH 值为 6.5 时会出现辉锑矿沉淀,因此没有对 Al 的相应参数进行评估。在溶解元素和 pH 值方面,发现生物钛铁矿的溶解是不协调的(非化学计量)。在 pH 值为 4 时,八面体层元素 Fe 的溶解占主导地位,而在 pH 值为 6.5 时,四面体元素 Si 的溶解占主导地位。没有证据表明形成了次生相,而且生物钛铁矿的沥滤速率与之前在有氧条件下进行的研究报告一致。此外,在实验前后,生物岩的铁(III)/Fetot 比率基本保持不变。这表明,尽管厌氧条件可能会影响蛭石的形成,但它本身对生物岩溶解的速率和性质影响不大。因此,以前在有氧条件下获得的生物岩溶解速率在厌氧条件下也可能有效。
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Biotite dissolution kinetics at pH 4 and 6.5 under anaerobic conditions and the release of dissolved Fe(II)

Dissolution of biotite, the main Fe-bearing mineral in granitic bedrock, is of particular importance for the remediation of reducing conditions after the ingress of oxygen, such as after mining activities or the construction of deep repositories for toxic waste. This study investigated the leaching of biotite of size fraction 0.053–0.075 mm under anaerobic conditions at room temperature and pH 4 and 6.5 for a maximum of 160 days. The changes in the concentrations of the major elements in the leaching solutions were monitored. In addition, Fe(II) was analysed separately. pH-independent rate coefficients kH+ were 4.8∙10−10, 6.9∙10−10, 6.3∙10−11, and 1.0∙10−12 mol1-n m−2 s-1, for Fe, Fe(II), Mn, and Si, respectively. The corresponding proton reaction orders nH+ were 0.61, 0.63, 0.33, and 0.09, respectively. The corresponding parameters for Al were not evaluated because of a suspected gibbsite precipitation at pH 6.5. The dissolution of biotite was found to be incongruent (non-stoichiometric) with respect to both the dissolving elements and the pH value. At pH 4, the dissolution was dominated by the octahedral layer element Fe, whereas at pH 6.5, the dissolution of the tetrahedral element Si dominated. There was no evidence of secondary phase formation, and the biotite leaching rates were consistent with those reported in previous studies conducted under aerobic conditions. In addition, the Fe(III)/Fetot ratio of biotite remained essentially unchanged before and after the experiment. This indicates that the anaerobic conditions alone have little effect on the rate and nature of biotite dissolution, although they may influence vermiculite formation. Therefore, biotite dissolution rates previously obtained under aerobic conditions may also be valid under anaerobic conditions.

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来源期刊
Chemical Geology
Chemical Geology 地学-地球化学与地球物理
CiteScore
7.20
自引率
10.30%
发文量
374
审稿时长
3.6 months
期刊介绍: Chemical Geology is an international journal that publishes original research papers on isotopic and elemental geochemistry, geochronology and cosmochemistry. The Journal focuses on chemical processes in igneous, metamorphic, and sedimentary petrology, low- and high-temperature aqueous solutions, biogeochemistry, the environment and cosmochemistry. Papers that are field, experimentally, or computationally based are appropriate if they are of broad international interest. The Journal generally does not publish papers that are primarily of regional or local interest, or which are primarily focused on remediation and applied geochemistry. The Journal also welcomes innovative papers dealing with significant analytical advances that are of wide interest in the community and extend significantly beyond the scope of what would be included in the methods section of a standard research paper.
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