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首页> 外文期刊>Environmental Science & Technology >Interfacial Energies for Heterogeneous Nucleation of Calcium Carbonate on Mica and Quartz
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Interfacial Energies for Heterogeneous Nucleation of Calcium Carbonate on Mica and Quartz

机译：云母和石英上碳酸钙非均相成核的界面能

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摘要

Interfacial free energies often control heterogeneous nucleation of calcium carbonate (CaCO_3) on mineral surfaces. Here we report an situ experimental study of CaCO_3 nucleation on mica (muscovite) and quartz, which allows us to obtain the interfacial energies governing heterogeneous nucleation. In situ grazing incidence small-angle X-ray scattering (GISAXS) was used to measure nucleation rates at different supersaturations. The rates were incorporated into classical nucleation theory to calculate the effective interfacial energies (α′)- Ex situ Raman spectroscopy identified both calcite and vaterite as CaCO_3 polymorphs; however, vaterite is the most probable heterogeneous nuclei mineral phase. The α′ was 24 mJ/m~2 for the vaterite-mica system and 32 mJ/m~2 for the vaterite-quarta system. The smaller α′ of the CaCO_3-mica system led to smaller particles and often higher parade densities on mica. A contributing factor affecting α′ in our system was the smaller structural mismatch between CaCO_3 and mica compared to that between CaCO_33 and quartz. The extent of hydrophilicity and the surface charge could not explain the observed CaCO_3 nucleation trend on mica and quartz. The findings of this study provide new thermodynamic parameters for subsurface reactive transport modeling and contribute to our understanding of mechanisms where CaCO_3 formation on surfaces is of concern.
机译：界面自由能通常控制矿物表面碳酸钙（CaCO_3）的异质成核。在这里，我们报告了在云母和白云母和石英上进行CaCO_3成核的原位实验研究，这使我们能够获得控制异质成核的界面能。原位掠入射小角度X射线散射（GISAXS）用于测量不同过饱和度下的成核率。将该比率纳入经典成核理论以计算有效界面能（α'）-非原位拉曼光谱法将方解石和球ate石均确定为CaCO_3多晶型物；然而，球ate石是最可能的非均质核矿物相。对于球ate石-云母系统，α'为24 mJ / m〜2，对于球v石-石英系统，α'为32 mJ / m〜2。 CaCO_3-云母系统的较小α'导致较小的颗粒，并且云母上的游行密度通常较高。影响我们系统中α'的一个因素是，CaCO_3和云母之间的结构失配比CaCO_33和石英之间的结构失配更小。亲水程度和表面电荷不能解释在云母和石英上观察到的CaCO_3成核趋势。这项研究的发现为地下反应性输运模型提供了新的热力学参数，并有助于我们理解其中关注表面CaCO_3形成的机理。

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  • 来源
    《Environmental Science & Technology》 |2014年第10期|5745-5753|共9页
  • 作者

    Qingyun Li; Alejandro Fernandez-Martinez; Byeongdu Lee; Glenn A Waychunas; Young-Shin Jun;

  • 作者单位

    Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, Missouri 63130,United States;

    CNRS, ISTerre, F-38041 Grenoble, France,Universite de Grenoble Alpes, ISTerre, F-38041 Grenoble, France;

    Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States;

    Earth Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States;

    Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, Missouri 63130,United States;

  • 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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