玄武岩CO2封存地球化学研究进展:微观机制与反应路径

Advances in research on geochemistry of CO2 storage in basalts: Microscopic mechanisms and reaction pathways

  • 摘要:
    目的和方法 全球温室气体减排的迫切需求推动了玄武岩CO2矿化封存技术的发展。为了进一步理解矿化过程的微观机制和反应路径,系统梳理过程中的地球化学反应机制,深入探讨超临界CO2与溶解态CO2注入下的反应路径差异、矿物溶解与碳酸盐沉淀的耦合关系,以及影响反应的关键因素。
    进展 超临界CO2注入通过纳米级水化层的多步骤耦合反应实现矿化,而溶解态注入则依赖于溶液相中的化学溶解和配位反应。在CO2玄武岩矿化反应中,橄榄石、辉石等矿物主导了金属阳离子的释放,而方解石、菱镁矿、铁白云石等碳酸盐矿物则在不同温压条件下依次沉淀。方解石沉淀具有宽温适应性,铁白云石和菱镁矿多见于中高温条件。pH、温度、CO2分压、流体盐度及岩石非均质性等因素对反应路径和沉淀矿物演化具有显著影响。较低的pH促进初生矿物的溶解,而较高的pH则有利于碳酸盐矿物的沉淀。高温有助于矿物溶解,提高反应速率。较高的CO2分压可增加CO2的溶解度和反应活性,进而加速矿物溶解和碳酸盐的形成。流体盐度通过改变溶液的离子强度和化学组成,影响矿物的溶解和沉淀过程。岩石的非均质性,包括矿物组成和孔隙结构差异,影响流体的运移路径和反应效率,促进局部沉淀和优先流动通道形成,可在低流量和非连通通道实现持续沉淀,未来需研究其对储层物性的影响。这些因素相互作用,共同决定CO2矿化封存的动态变化过程。
    展望 鉴于此,在综述玄武岩中CO2矿化过程的基础上,提出了未来研究方向,包括构建参数优化框架、发展高分辨率耦合模型及优化注入策略,以推动玄武岩CO2封存技术的规模化应用与工程落地。深入研究反应影响因素的协同作用机制,将为优化封存技术提供更坚实的理论基础,进一步提高CO2矿化封存的效率和稳定性。

     

    Abstract:
    Objective and Methods  The urgent need to reduce global greenhouse gas emissions has driven the development of CO2 mineral trapping in basalts. To gain further insights into the microscopic mechanisms and reaction pathways of the mineral trapping, this study systematically reviews the geochemical reaction mechanisms involved, with a particular focus on the differences in reaction pathways between supercritical and dissolved CO2 injection, the coupling between mineral dissolution and carbonate precipitation, and the key factors influencing these reactions.
    Advances  In the case of supercritical CO2 injection, CO2 mineral trapping is achieved through multi-step coupling reactions in nanoscale hydration layers. Under dissolved CO2 injection, the mineral trapping is primarily achieved through chemical dissolution and coordination reactions in the aqueous phase. In the geochemical reactions during CO2 mineral trapping in basalts, minerals such as olivine and pyroxene play a dominant role in the release of metal cations, while carbonate minerals including calcite, magnesite, and ankerite precipitate sequentially under different temperature and pressure conditions. Calcite exhibits broad temperature adaptability, whereas magnesite and ankerite are commonly observed under moderately high temperature conditions. Factors such as pH, temperature, CO2 partial pressure ( p_\textC\textO_\text2 ), fluid salinity, and rock heterogeneity exert significant impacts on reaction pathways and the evolution of minerals precipitated. Specifically, low pH accelerates the dissolution of primary minerals, while high pH creates favorable conditions for the precipitation of carbonate minerals. Elevated temperatures promote mineral dissolution, thus increasing the reaction rates. High CO2 partial pressure can enhance the solubility and reactivity of CO2, thereby accelerating mineral dissolution and carbonate formation. Fluid salinity affects the dissolution and precipitation processes of minerals by changing the ionic strength and chemical composition of solutions. Rock heterogeneity, including differences in mineral compositions and pore structures, affects fluid transport pathways and reaction efficiency. Furthermore, it facilitates localized precipitation and the formation of preferential flow channels, enabling sustained precipitation in low-flow and disconnected channels. It is necessary to investigate the impacts of rock heterogeneity on reservoir physical properties in the future. The abovementioned factors interact with each other, jointly determining the dynamic evolution of CO2 mineral trapping.
    Prospects  Future research directions are proposed in this study based on the review, including the establishment of parameter optimization frameworks, the construction of high-resolution coupling models, and the optimization of CO2 injection strategies. These efforts will promote the large-scale applications and engineering implementation of CO2 storage in basalts. Additionally, a thorough investigation into the mechanisms behind the synergy among the influential factors of reactions will lay a solid theoretical foundation for the optimization of CO2 storage technology, thus further improving the efficiency and stability of CO2 mineral trapping.

     

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