Synergistic Effects of Cyanobacteria and Montmorillonite on Formation of Low-Temperature Protodolomite
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摘要: 白云石[CaMg（CO3）2]的成因机制是地球科学领域长期关注的重要问题.尽管已有研究表明特定微生物功能群和黏土矿物能够分别催化原白云石（有序白云石的关键前驱体）的形成，然而对于蓝细菌这一古老且广泛分布的光合微生物的催化作用，特别是其与黏土矿物的协同效应机制，目前仍缺乏深入认识.研究以耐盐蓝细菌Synechococcus elongatus FACHB⁃410为研究对象，通过对比有无蒙脱石的矿化实验体系，探究了黏土矿物与蓝细菌对碳酸盐矿物沉淀的协同调控作用.实验结果表明，在蓝细菌—蒙脱石共存体系中，X⁃射线衍射（X⁃ray diffraction，XRD）和拉曼光谱证实主要形成原白云石，而不含蒙脱石的体系则生成单水方解石和低镁方解石.通过扫描电镜（scanning electron microscopy，SEM）、聚焦离子束显微镜（focused ion beam microscopy，FIB⁃SEM）和透射电镜（transmission electron microscopy，TEM）等表征技术，发现原白云石以纳米晶粒形式组装并分布于蒙脱石表面.基于密度泛函理论（density functional theory，DFT）的计算模拟进一步表明，蒙脱石促进蓝细菌介导原白云石形成的关键机制在于其表面负电性，即通过强静电作用吸附水合镁离子，有利于其去水合化反应的发生，从而显著降低原白云石的成核能垒.Abstract: The formation mechanism of dolomite [CaMg(CO3)2] remains a longstanding enigma in earth sciences. Previous studies have identified certain microorganisms and clay minerals as catalysts in the crystallization of low-temperature protodolomite, a crucial precursor to ordered dolomite. However, the role of cyanobacteria and particularly their potential synergistic effects with clay minerals remain poorly understood. In this study, we investigated bioprecipitation of carbonate minerals using the halotolerant cyanobacterium Synechococcus elongatus FACHB-410 in the presence and absence of montmorillonite. Our results demonstrated that protodolomite occurred as the predominant solid product in the montmorillonite-amended biosystems as confirmed by X-ray diffraction (XRD) and Raman spectroscopy, whereas monohydrocalcite and low-magnesian calcite were the primary products in the montmorillonite-free biosystems. Multiple microscopic techniques, including scanning electron microscopy (SEM), focused ion beam microscopy (FIB-SEM), and transmission electron microscopy (TEM), revealed that protodolomite nucleated as nanocrystals preferentially on montmorillonite surfaces. Density functional theory (DFT) simulations further elucidated that surface electronegativity of montmorillonite played a key role in promoting protodolomite formation by strongly adsorbing Mg2+ ions through electrostatic interactions, thereby facilitating their dehydration and significantly lowering the nucleation energy barrier.
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Key words:
- dolomite problem /
- clay minerals /
- protodolomite /
- cyanobacteria /
- microbial mineralization
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图 1 有无蒙脱石条件下蓝细菌矿化产物的XRD图谱
a.全谱图；b.28°~33° 2θ局部放大
Fig. 1. XRD patterns of precipitates from the bioreactors with and without montmorillonite
图 2 蒙脱石存在条件下蓝细菌矿化产物形貌(a)及拉曼图谱(b)
Fig. 2. Light microscopic photograph (a) and raman spectra (b) of precipitates from the bioreactors with montmorillonite
图 3 未添加蒙脱石的体系中蓝细菌矿化产物的SEM图像
Fig. 3. SEM images of precipitates from bioreactors without montmorillonite
图 4 蒙脱石存在条件下蓝细菌矿化体系产物的SEM图像
Fig. 4. SEM images of precipitates from bioreactors with montmorillonite
图 5 蒙脱石条件下蓝细菌矿化反应体系产物的FIB⁃SEM-EDS图谱
a.蒙脱石-原白云石聚集体，其中虚线显示切割位置；b~e.蒙脱石-原白云石聚集体切割面及Ca、Mg、Si元素分布
Fig. 5. FIB⁃SEM and EDS images of precipitates from bioreactors with montmorillonite
图 6 黏土矿物存在条件下反应体系最终产物的TEM分析
a~c.蒙脱石-原白云石聚集体，其中b和c的插图分别显示了蒙脱石的高分辨晶格条纹以及原白云石的电子衍射谱；d.原白云石（113）晶面的高分辨晶格条纹；e~h.蒙脱石-原白云石聚集体的元素分布图，其中f、g和h分别对应Ca、Mg和Si的元素分布；i沿e中实线扫描路径获得的原白云石颗粒中Ca和Mg元素的EDS线扫描分布
Fig. 6. TEM images of precipitates from reactors with clay minerals
图 7 DFT模拟蒙脱石水合镁离子的吸附过程
a.蒙脱石表面差分电荷图；b.羟基位点与水合镁离子的配位构型
Fig. 7. DFT simulation showing the adsorption process of Mg(H2O)62+ on the montmorillonite (010) surface
图 8 蓝细菌-蒙脱石协同介导原白云石形成过程的示意
Fig. 8. Schematic illustration of protodolomite formation mediated synergistically by cyanobacteria and montmorillonite
表 1 有无蒙脱石矿物条件下反应体系的水化学参数变化
Table 1. Wet chemistry parameter changes in the biomineralization systems with and without montmorillonite
实验体系 开始培养 结束培养(30 d) pH值 Ca2+ (mmol/L) Mg2+ (mmol/L) pH值 Ca2+ (mmol/L) Mg2+ (mmol/L) 蓝细菌 7.20±0.01 10.05±0.03 80.87±0.21 9.58±0.11 1.35±0.09 78.86±0.43 蓝细菌+蒙脱石 7.21±0.02 10.03±0.06 78.96±0.18 9.27±0.06 1.74±0.13 71.05±0.25 
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