The mechanism of inorganic carbon sink in the stabilization process of Zn2+ contaminated red clay in karst area
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摘要: 岩溶区高镁地质背景赋予其天然无机碳汇潜力，但长期铅锌矿采选导致的Zn2+污染严重削弱该功能，且传统固化/稳定化（S/S）技术高碳排放、长期稳定性差，难以实现低碳环保的目标。本研究提出采用活性MgO强化CO2无机碳汇固稳技术治理岩溶区Zn2+污染红黏土，系统考察了Zn2+污染浓度、活性MgO掺量及反应时间对Zn2+固稳效果的影响，并通过BCR顺序提取、XRD和SEM揭示固稳机制。结果表明：提高活性MgO掺量并优化反应时间可显著降低游离态Zn2+含量，促进其向残渣态转化。水合碳酸镁（HMCs）为主要碳汇产物，通过活性MgO与CO2反应实现高效CO2矿化封存，同时对Zn2+产生包裹吸附及胶结填充作用，形成稳定碳酸盐矿物结构，实现Zn2+固稳与人工无机碳汇的协同。本研究揭示了该技术在岩溶区Zn2+污染红黏土固稳中的微观机制，为岩溶地区重金属污染治理与实现碳中和目标提供了新路径。Abstract:
The karst area exhibits both ecological vulnerability and hydrogeological complexity. The unique carbonate landform and the high-permeability underground runoff characteristics make pollutants spread rapidly. Long-term lead-zinc mining and processing have led to continuous accumulation of soil heavy metal pollution in karst areas, especially severe Zn2+ accumulation in red clay, which destroys soil structure and significantly weakens the potential of natural inorganic carbon sinks in the region. At the same time, it causes compound soil-groundwater pollution, surface subsidence, and other geological disasters. Traditional solidification/stabilization (S/S) technology mainly relies on materials such as cement and lime. Although it can reduce the leaching risk of heavy metals to some extent, it still has problems such as high carbon emissions, poor long-term stability, and a long construction period. It is difficult to achieve the goal of low carbon and environmental protection. It cannot meet the needs of green restoration in the complex karst environment. To address the above problems, this study proposes an active MgO-enhanced CO2 inorganic carbon sink stabilization technology as a green, low-carbon remediation approach. This technology mainly uses low-temperature-prepared active MgO as a curing material to generate hydrated magnesium carbonate (HMCs) through an inorganic carbon sink reaction in a CO2 environment, thereby stabilizing heavy metals and advancing the development of artificial inorganic carbon sinks. Compared with traditional high-temperature calcined MgO, active MgO has the advantages of a large specific surface area, high reactivity, and low energy consumption, and can be better utilized in the geological background of high magnesium in karst areas. In this study, the typical Zn2+-contaminated red clay in a karst area was taken as the research object. The effects of Zn2+ pollution concentration, active MgO content, and reaction time on Zn2+ stabilization were systematically investigated. The morphological transformation of Zn2+ was analyzed using the BCR sequential extraction method; phase identification was performed by X-ray diffraction (XRD); and the morphology of the reaction products and the evolution of soil microstructure were observed by scanning electron microscopy (SEM) to reveal the stabilization mechanism. The results show that increasing the content of active MgO and optimizing the reaction time can increase the sample's resistivity, significantly reduce the free Zn2+ content, and promote its conversion to a residual state. A large amount of hydrated magnesium carbonate (HMCs), such as hydromagnesite, spherulite, and trihydrate magnesite, is generated as the main carbon sink products. High-efficiency CO2 mineralization and storage can be achieved by reacting active MgO with CO2. At the same time, the adsorption and cementation of Zn2+ can form a stable carbonate mineral structure, and the coordination of Zn2+ stabilization and an artificial inorganic carbon sink can be achieved. Unlike the high carbon-emission characteristics of traditional solidification/stabilization (S/S) technology, this study focuses on the key constraint posed by a high-magnesium geological background in a karst area. It extends the active MgO-enhanced CO2 inorganic carbon sink technology to the remediation of Zn2+ contaminated red clay. Through systematic research, the mechanism of action of hydrated magnesium carbonate (HMCs) in mediating heavy metal stabilization at the micro level is clarified, providing a new theoretical explanation and technical path for the green, low-carbon treatment of heavy metal pollution in karst areas and the realization of carbon neutrality goals. In addition to discussing the variation in the influence of different factors on the stabilization effect and carbon sink mechanism, this study also guides engineering restoration of complex geological environments in karst areas. The technology offers fast reaction speed, excellent stabilization, significant environmental benefits, and strong carbon-sink potential. It shows broad application prospects for addressing heavy metal pollution in karst areas, reducing geological disasters, and advancing carbon neutrality. The active MgO-enhanced CO2 inorganic carbon sequestration stabilization technology proposed in this study has significant green and low-carbon advantages. The current research is mainly based on laboratory experiments. In the future, it is necessary to further conduct relevant model tests or on-site long-term monitoring to comprehensively evaluate the long-term stability, ion migration laws, and actual CO2 sequestration efficiency of the technology, thereby promoting its practical application in the remediation of contaminated sites in karst areas. In summary, this study demonstrates significant potential for sustainable and ecological restoration of the fragile karst ecosystem through the active MgO-enhanced CO2 inorganic carbon sink stabilization technology, providing new ideas and methods for low-carbon, efficient restoration of Zn2+ contamination in karst areas. It has important scientific significance and engineering value in promoting the coordinated development of heavy metal pollution control and artificial carbon sinks. -
Key words:
- Karst area /
- Inorganic carbon sink /
- Red clay /
- Zn2+ contaminated soil /
- Stabilization mechanism
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图 2 不同变量对固稳污染红黏土的应力-应变曲线
Figure 2. Stress-strain curves of different variables on stabilized contaminated red clay
图 3 活性MgO强化CO2无机碳汇固化Zn2+污染土电阻率随应变变化规律
Figure 3. The variation of resistivity of Zn2+ contaminated soil solidified by CO2 inorganic carbon sink enhanced by active MgO with strain
图 4 活性MgO强化CO2无机碳汇固化Zn2+污染土的电阻率与活性MgO掺量和反应时间拟合曲线
Figure 4. Fitting curves of resistivity of Zn2+ contaminated soil solidified by CO2 inorganic carbon sink enhanced by reactive MgO with reactive MgO content and reaction time
图 5 活性MgO强化CO2无机碳汇固稳Zn2+形态分布
Figure 5. Distribution of heavy metal species in CO2 inorganic carbon sequestration enhanced by active MgO
图 6 不同活性MgO掺量(a)以及不同反应时间(b)Zn2+污染土XRD图谱
Figure 6. XRD patterns of Zn2+ contaminated soil with different active MgO content ( a ) and different reaction time ( b )
图 7 不同活性MgO掺量下固化Zn2+污染土的SEM图
Figure 7. SEM images of solidified Zn2+ contaminated soil with different active MgO content
图 8 不同反应时间下活性MgO强化CO2无机碳汇固稳Zn2+污染土的SEM图
Figure 8. SEM images of active MgO reinforced CO2 inorganic carbon sequestration and stabilized Zn2+ contaminated soil under different reaction time
表 1 红黏土的基本物性指标
Table 1. Basic physical properties of red clay
最优含水率
ω/%最大干密度
ρd/g∙cm−3比重GS 液限
WL/%塑限
WP/%塑性指数
IP30.00 1.49 2.73 57.95 31.22 26.73 
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表 2 六水合硝酸锌(Zn(NO3)2 ∙6H2O)（分析纯）技术条件表（单位：%）
Table 2. Technical conditions of zinc nitrate hexahydrate (Zn(NO3)2·6H2O) (analytically pure) ( unit : % )
化合物 [Zn(NO3)2 6H2O] pH值 水不
溶物氯化物
(Cl−)硫酸根
(${\rm{SO}}_4^{2-}$)铁
(Fe3+)铅
(Pb2+)硫化铵
不沉淀物含量 ≥99.0 ≥3.5 0.005 0.001 0.002 0.0003 0.005 0.10 （注：pH值是在溶解度为50 g/L，温度25 ℃下测定的）
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表 3 活性MgO化学组成表（%）
Table 3. Active MgO chemical composition table (%)
成分 K2O MgO MnO Na2O P2O5 Al2O3 CaO Fe2O3 SiO2 其他 含量 — 93.20 0.02 0.23 0.08 0.16 1.80 0.04 0.61 2.5
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表 4 活性MgO强化无机碳汇固化Zn2+污染土试验方案
Table 4. Experimental scheme of solidified Zn2+ contaminated soil by active MgO enhanced inorganic carbon sink
Zn2+浓度ic/% 活性MgO掺量M/% 碳化时间t/h 试验内容 500 mg∙kg−1 2.5 0.5 无侧限抗压强度- 1000 mg∙kg−15 1 电阻率测试 5000 mg∙kg−17.5 3 BCR测试 10000 mg∙kg−110 6 XRD测试 12 SEM测试
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