从晶体成核—生长热动力学剖析白云岩成因问题的新进展

doi:10.13745/j.esf.sf.2025.3.71

摘要/Abstract

摘要：

“白云岩问题”已持续困扰了地质学家200余年,无疑是地质学上争议最长久的难题之一。为推进白云岩成因问题的研究,本文借助晶体结构分析对白云岩晶体结构特征进行差异性研究,明确其形成环境及演化特征,进而为揭示其成因机制提供依据。由于晶体结构和成核-生长动力学之间存在相互影响和制约的关系,本文将晶体结构研究与成核-生长热动力学理论相结合,深入剖析白云岩的形成机制和条件。晶体结构分析表明,晶体结构控制了白云石的晶体类型、成核-生长速率、生长方向和其晶体最终形态,并决定了其热力学和动力学性质。热力学研究表明,现代海水具有析出白云石的热力学倾向,白云化反应可以在标准状态下进行,然而现代海水白云石的沉积量非常有限,建立新的热力学模型解释白云岩成因问题仍需结合实际加以验证可行性。动力学研究表明,海水中低温无机白云石形成困难的动力学因素包括Mg²⁺的水合作用、硫酸盐、阳离子有序化过程、$\mathrm{CO}_{3}^{2-}$的活性、溶液过饱和度和成核位点的有无等。但对于这些因素研究的认识仍然存在分歧,并没有解决低温无机白云石形成的关键问题。白云岩的形成和有序化是在地质时期内溶解-重结晶的结果,白云岩早期阶段可能受成核动力学控制,产物以亚稳定中间相为主,而后主要是受生长动力学控制。高新技术的发展与应用,使矿物学研究向分子、原子尺度深入,为白云石形成机制的研究提供方向。因此,合理利用高新技术,结合晶体结构分析和晶体成核-生长热动力学理论,从原子尺度探索白云石晶体生长机制,以期为研究白云岩成因提供新视角,进而为解开白云岩成因之谜提供重要的理论和实验基础。

关键词: 白云岩成因, 晶体结构, 晶体成核-生长, 热力学, 动力学

Abstract:

The “Dolomite Problem” has been a source of contention among geologists for over two centuries and remains one of the most contentious issues in the field. To advance research on dolomite genesis, this paper employs crystal structure analysis to investigate its structural characteristics, formation environment, and evolutionary characteristics, thereby providing a basis for revealing its formation mechanism. Given the mutual influence and constraints between crystal structure and nucleation-growth kinetics, the study combines crystal structure analysis with nucleation-growth thermodynamics to analyze dolomite’s formation mechanism and conditions in detail. Results demonstrate that the crystal structure controls the mineral type, nucleation-growth rate, growth direction, and final morphology of dolomite, thus determining its thermodynamic and kinetic properties. Thermodynamic studies indicate that modern seawater exhibits a thermodynamic tendency to precipitate dolomite, and the dolomitization reaction can proceed under standard conditions. However, actual dolomite deposition in modern seawater is minimal, and the feasibility of establishing a new thermodynamic model to explain dolomite genesis requires verification through experimentation. Kinetic studies reveal that factors impeding low-temperature inorganic dolomite formation in seawater include Mg²⁺ hydration, sulfate effects, cation ordering processes, $\mathrm{CO}_{3}^{2-}$ activity, solution supersaturation, and the presence or absence of nucleation sites. Nevertheless, current understanding of these factors remains inconclusive and does not fully resolve the pivotal issue of low-temperature inorganic dolomite formation. Dolomite formation and ordering result from dissolution-recrystallization processes over geological time. In the initial stages, dolomite formation is likely controlled by nucleation kinetics, with metastable intermediate phases predominating. As the process advances, growth kinetics becomes the primary control. The development and application of advanced analytical techniques have facilitated mineralogical research at the molecular and atomic scales. Such analysis provides direction for studying dolomite formation mechanisms. We therefore recommend utilizing advanced techniques rationally, integrating crystal structure analysis and nucleation-growth thermodynamic theory, to explore dolomite crystal growth mechanisms at the atomic scale. This approach aims to furnish novel perspectives on dolomite genesis research and provide a robust theoretical and empirical foundation for potentially unraveling the enigma of dolomite formation.

Key words: dolomite genesis, crystal structure, crystal nucleation-growth, thermodynamics, kinetics

中图分类号:

高和婷, 李茜, 朱光有, 李生, 王瑞林, 侯佳凯, 张杰志, 郑凯航. 从晶体成核—生长热动力学剖析白云岩成因问题的新进展[J]. 地学前缘, 2025, 32(5): 165-189.

GAO Heting, LI Xi, ZHU Guangyou, LI Sheng, WANG Ruiling, HOU Jiakai, ZHANG Jiezhi, ZHENG Kaihang. A review of dolomite genesis analysis based on crystal nucleation-growth thermodynamic and kinetic[J]. Earth Science Frontiers, 2025, 32(5): 165-189.

图/表 19

图1 白云石晶胞模型(据文献[13]修改)

Fig.1 Dolomite crystal structure. Modified after [13].

图2 白云石的X射线衍射谱图及超结构衍射线(015),(021)和(101)(据文献[13]修改) a—理想白云石X射线衍射谱图及超结构衍射线;b—无机原白云石X射线衍射谱图及超结构衍射线。

Fig.2 X-ray diffraction pattern and superstructure diffraction lines of dolomite (015), (021), and (101). Modified after [13].

表1 晶体结构参数特征表

Table 1 Characterisation of crystal structure parameters

晶体结构参数	含义	表示符号/类型	指示意义
有序度	晶体中原子排列有序的情况	δ=I(015)/I(110),有序度越高,晶体生长过程中的环境条件越稳定,反之则可能表示环境条件的剧烈变化	指示形成环境、流体来源、成因、成岩演化和石油地质研究
晶胞参数	晶体中最小的单元	a、b、c,微量元素的混入会改变参数值,理想白云石的a=b=4.806 9 Å,c=16.003 4 Å	直接反映晶体中结构特征,判断白云石晶体形成环境
晶面间距	晶体中相邻晶面之间的距离	d,通常会计算d₁₀₄晶面间距	判断白云石的形成环境和成因
晶格缺陷	晶体中原子排列不规则的现象	点缺陷、线缺陷、面缺陷和体缺陷	反映晶体形成环境、形成和生长过程

表2 不同类型白云石晶体结构参数与其形成环境关系

Table 2 Correlation of crystalline structure parameters of diverse dolomite types with their respective formation environments

白云石类型	晶体结构参数特征	沉积环境	研究实例
原生沉积白云石	晶形相对规则,多呈自形-半自形;晶体粒度以泥晶-粉晶为主,一般泥晶白云石粒度小于4 μm,粉晶白云石粒度在4~10 μm;有序度较差,一般在0.3~0.6之间;晶胞参数接近理想白云石值(a=4.80 Å,c=16.02 Å);晶面间距较大,且稳定;晶体结构较为完整,晶格缺陷较少。	指示其在相对稳定、低能的沉积环境中形成,如温暖浅海、盐湖等沉积环境。	[2,13,19,20, 56,74,77,78, 86-92]
次生交代白云石	晶形常不规则,多为它形;晶体粒度变化大,可从细晶到粗晶,常见中-粗晶(大于10 μm);有序度值较高,一般在0.8~1.0之间;晶胞参数偏离理想值,a值可能增大或减小,c值也会相应改变;晶面间距变化差异大;存在较多晶格缺陷。	指示其形成受后期热液、卤水等交代作用影响而形成,如热液活动频繁区域、岩浆岩与围岩接触带和断裂构造附近。	[72,76,79-85]

图3 结晶过程图(据文献[93]修改)

Fig.3 Crystallization diagram of crystallization process. Modified after [93].

表3 动力学制约因素

Table 3 Kinetic constraints

动力学制约因素	制约机理	研究进展
Mg²⁺的水合作用	Mg²⁺与水分子具有强键合作用,形成Mg²⁺水化壳,阻碍白云石生长。	类白云石矿物并未受到Mg²⁺水合作用的障碍,需重新评估Mg²⁺水合作用对白云石形成动力学制约情况。
溶液中$\mathrm{CO}_{3}^{2-}$ 的活性	$\mathrm{CO}_{3}^{2-}$的含量极低,且只有极少数$\mathrm{CO}_{3}^{2-}$具有足够的动能穿透水化屏障,溶液中$\mathrm{CO}_{3}^{2-}$的活性会限制白云石的形成。	微生物、热化学的硫酸盐的还原反应可生成$\mathrm{CO}_{3}^{2-}$/$\mathrm{HCO}_{3}^{-}$,致使环境的碳酸盐碱度增加,有利于白云岩形成。$\mathrm{CO}_{3}^{2-}$的活性并不是导致白云石形成困难的主控因素。
硫酸盐	$\mathrm{SO}_{4}^{2-}$和Mg²⁺会形成紧密的Mg_xSO₄离子对,导致进入晶格中的Mg²⁺减少,阻碍继续白云石生长。	在低温下硫酸盐的抑制作用被高估,$\mathrm{SO}_{4}^{2-}$可起到催化作用促进白云石沉淀。
过饱和度	过饱和条件会形成有序层,晶体在长期过饱和条件下这些有序层无法再生长。	沉积体系中水化学的动荡过程(饱和-不饱和、盐度或pH波动等)是近地表有序白云石形成的有利条件。
阳离子有序化过程	有序化过程中低温条件溶液的Ca²⁺、Mg²⁺和$\mathrm{CO}_{3}^{2-}$迁移至特定的晶格位置的速率很缓慢,限制了白云石有序生长的能力。	在白云石的早期生长阶段就可能存在某种程度的有序化。低温下较短时间内可生成一些类白云石结构矿物,且具备有序结构,缓慢阳离子有序化过程是否为抑制白云石形成的动力学因素还需进一步商榷。
成核位点	成核位点的有无决定了白云石在低温条件下的成核率。	微生物细胞表面也可为白云石的沉淀提供成核位点,也有学者发现细菌很难为矿物形成提供成核位点,仍需对微生物在低温白云石形成中的作用进行深入评估。
成核动力学	团簇临界尺寸自由能屏障控制成核速率。	白云石的成核势垒比方解石和文石的成核势垒低,白云石晶核加入显著缩短了白云化作用的时间,促进了白云石的生长,表明白云石的成核不受限制。
生长动力学	晶体生长方式(层生长、螺旋位错生长等)提供的生长位点,决定晶体生长速率。	在过饱和度和欠饱和度之间进行周期性的频繁切换可以加速白云石的生长。证明了溶解-重结晶合成有序白云石的方法是可行的,这为低温无机成因白云岩的形成提供了新思路。

表3 动力学制约因素

Table 3 Kinetic constraints

动力学制约因素	制约机理	研究进展
Mg²⁺的水合作用	Mg²⁺与水分子具有强键合作用,形成Mg²⁺水化壳,阻碍白云石生长。	类白云石矿物并未受到Mg²⁺水合作用的障碍,需重新评估Mg²⁺水合作用对白云石形成动力学制约情况。
溶液中$\mathrm{CO}_{3}^{2-}$ 的活性	$\mathrm{CO}_{3}^{2-}$的含量极低,且只有极少数$\mathrm{CO}_{3}^{2-}$具有足够的动能穿透水化屏障,溶液中$\mathrm{CO}_{3}^{2-}$的活性会限制白云石的形成。	微生物、热化学的硫酸盐的还原反应可生成$\mathrm{CO}_{3}^{2-}$/$\mathrm{HCO}_{3}^{-}$,致使环境的碳酸盐碱度增加,有利于白云岩形成。$\mathrm{CO}_{3}^{2-}$的活性并不是导致白云石形成困难的主控因素。
硫酸盐	$\mathrm{SO}_{4}^{2-}$和Mg²⁺会形成紧密的Mg_xSO₄离子对,导致进入晶格中的Mg²⁺减少,阻碍继续白云石生长。	在低温下硫酸盐的抑制作用被高估,$\mathrm{SO}_{4}^{2-}$可起到催化作用促进白云石沉淀。
过饱和度	过饱和条件会形成有序层,晶体在长期过饱和条件下这些有序层无法再生长。	沉积体系中水化学的动荡过程(饱和-不饱和、盐度或pH波动等)是近地表有序白云石形成的有利条件。
阳离子有序化过程	有序化过程中低温条件溶液的Ca²⁺、Mg²⁺和$\mathrm{CO}_{3}^{2-}$迁移至特定的晶格位置的速率很缓慢,限制了白云石有序生长的能力。	在白云石的早期生长阶段就可能存在某种程度的有序化。低温下较短时间内可生成一些类白云石结构矿物,且具备有序结构,缓慢阳离子有序化过程是否为抑制白云石形成的动力学因素还需进一步商榷。
成核位点	成核位点的有无决定了白云石在低温条件下的成核率。	微生物细胞表面也可为白云石的沉淀提供成核位点,也有学者发现细菌很难为矿物形成提供成核位点,仍需对微生物在低温白云石形成中的作用进行深入评估。
成核动力学	团簇临界尺寸自由能屏障控制成核速率。	白云石的成核势垒比方解石和文石的成核势垒低,白云石晶核加入显著缩短了白云化作用的时间,促进了白云石的生长,表明白云石的成核不受限制。
生长动力学	晶体生长方式(层生长、螺旋位错生长等)提供的生长位点,决定晶体生长速率。	在过饱和度和欠饱和度之间进行周期性的频繁切换可以加速白云石的生长。证明了溶解-重结晶合成有序白云石的方法是可行的,这为低温无机成因白云岩的形成提供了新思路。

图4 阳离子水合作用阻碍白云岩形成示意图(据文献[112]修改)

Fig.4 Sketch map of strong hydration of cation preventing dolomite formation. Modified after [112].

图5 硫酸盐还原菌促进白云石形成的模式图(据文献[120]修改)

Fig.5 Schematic model showing role of sulphate-reducing bacteria in dolomite formation. Modified after [120].

图6 特定官能团破坏Mg2+水合作用的能量壁垒(据文献[90])

Fig.6 Specific functional groups can break the energy barrier of Mg2+ hydration. Adapted from [90].

图7 均相与非均相成核动力学模式(据文献[141-142]) a—从溶液中形成一个半径为r的球形原子核;b—自由能变化;c—在异质底物上形成半球形核。

Fig.7 Models of homogeneous and heterogeneous nucleation dynamics. Adapted from [141-142].

图8 经典成核理论的自由能与晶核半径关系示意图(据文献[138])

Fig.8 Schematic representation showing the dependence of nucleation barrier ΔGC on the radius rc based on classical nucleation theory. Adapted from [138].

图9 碳酸钙成核和结晶路径示意图(据文献[161-162]修改) a—经典成核;b—非经典成核(聚集);c—非经典成核(相变)。

Fig.9 Schematic illustration of nucleation and crystallization paths for CaCO3. Modified after [161-162].

图10 不同晶体生长模式(据文献[164]) a—“岛状生长”模式;b—“逐层生长”模式;c—“层岛式生长”模式。

Fig.10 Different models of crystal growth. Adapted from [164].

图11 晶体生长过程示意图(据文献[142]) a—晶体表面的原子过程;b—二维成核的自由能垒;c—位错丘的几何形状。

Fig.11 Schematic illustration of the crystal growth process. Adapted from [142].

图12 水和岩石化学的模拟和实验结果比较(据文献[72])

Fig.12 Comparison of simulation and experimental results for water and rock chemistry. Modified after [72].

图13 白云石晶体生长的原位液体电池TEM图像(据文献[43]) a—光束诱导溶解循环前的白云石晶体;b—3 840次溶解循环后的晶体;蓝色虚线(溶解循环前)和红色虚线(溶解循环后)表示通过图像对比分析量化的晶体边缘,蓝色和红色虚线表示晶体在3 840个溶解周期后向各个方向生长。根据方向的不同,每1 000个循环的生长速度从8 nm到30 nm不等;c—原位液池TEM实验示意图;d—从b中绿色虚线圆圈所示区域测量的电子衍射图,白色三角形所示的衍射点被归类为有序白云石(JCPDS 36-426)。

Fig.13 In situ liquid cell TEM images of dolomite crystal growth. Adapted from [43].

图14 显生宙和晚元古代百万年白云岩年龄与阳离子有序度的关系(据文献[19,52,75])

Fig.14 Cation order versus dolomite age in million years through the Phanerozoic and Late Proterozoic. Adapted from [19,52,75].

图15 方解石、白云石各晶面表面能与断键密度关系(据文献[166])

Fig.15 Relationship between surface energy and bond-breaking density of each crystal surface of calcite and dolomite. Adapted from [166].

图16 方解石、白云石的白云化、晶面、晶界溶解示意图(据文献[45]) a—BE、OE模型中Mg取代率对体积减少量的关系;b—BE和OE模型中Mg取代率与晶格应力的关系;c—白云石的边界模型。

Fig.16 Schematic illustration of calcite and dolomite dolomitisation, crystal faces, and grain boundary dissolution. Adapted from [45].

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