Stellan Holgersson , Henrik Drake , Andreas Karlsson , Lindsay Krall
{"title":"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","authors":"Stellan Holgersson , Henrik Drake , Andreas Karlsson , Lindsay Krall","doi":"10.1016/j.chemgeo.2024.122204","DOIUrl":null,"url":null,"abstract":"<div><p>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 <em>k</em><sub><em>H+</em></sub> were 4.8∙10<sup>−10</sup>, 6.9∙10<sup>−10</sup>, 6.3∙10<sup>−11</sup>, and 1.0∙10<sup>−12</sup> mol<sup>1-n</sup> m<sup>−2</sup> s<sup>-1,</sup> for Fe, Fe(II), Mn, and Si, respectively. The corresponding proton reaction orders <em>n</em><sub><em>H+</em></sub> 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)/Fe<sub>tot</sub> 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.</p></div>","PeriodicalId":9847,"journal":{"name":"Chemical Geology","volume":null,"pages":null},"PeriodicalIF":3.6000,"publicationDate":"2024-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0009254124002845/pdfft?md5=2c293d9f321911dd7438ba9ff08c9271&pid=1-s2.0-S0009254124002845-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Biotite dissolution kinetics at pH 4 and 6.5 under anaerobic conditions and the release of dissolved Fe(II)\",\"authors\":\"Stellan Holgersson , Henrik Drake , Andreas Karlsson , Lindsay Krall\",\"doi\":\"10.1016/j.chemgeo.2024.122204\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>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 <em>k</em><sub><em>H+</em></sub> were 4.8∙10<sup>−10</sup>, 6.9∙10<sup>−10</sup>, 6.3∙10<sup>−11</sup>, and 1.0∙10<sup>−12</sup> mol<sup>1-n</sup> m<sup>−2</sup> s<sup>-1,</sup> for Fe, Fe(II), Mn, and Si, respectively. The corresponding proton reaction orders <em>n</em><sub><em>H+</em></sub> 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)/Fe<sub>tot</sub> 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. 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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.
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.