1. 中国地质大学(武汉)环境学院
2. 中国科学院武汉岩土力学研究所,岩土力学与工程安全全国重点实验室
3. 武汉大学
网络首发:2024-11-27,
纸质出版:2025
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高启荣, 雷宏武, 蔡雨娜, 等. 高温高压条件下非纯CO2-水体系的pH原位测量和预测模型[J]. 地质科技通报, 2025,44(4):116-128. DOI: 10.19509/j.cnki.dzkq.tb20240421.
高启荣, 雷宏武, 蔡雨娜, et al. 高温高压条件下非纯CO2-水体系的pH原位测量和预测模型[J]. Bulletin of Geological Science and Technology, 2025, 44(4): 116-128. DOI: 10.19509/j.cnki.dzkq.tb20240421.
含CO
2
的气体注入到深部含水层中会溶解形成碳酸,导致含水层的pH值下降,进而造成矿物的溶解或沉淀,影响CO
2
地质利用与封存的安全性和有效性。p H值作为能表征溶液化学性质的重要参数,因此通过实验测量纯/非纯CO
2
饱和溶液体系的p H值,并结合模型预测可以评估CO
2
地质封存条件下的化学变化。在原位条件下通过电势法和光谱法测量了温度范围35~93℃、压力范围0.38~18 MPa时,纯CO
2
-H
2
O体系和非纯CO
2
-H
2
O体系的p H值;并建立了基于溶解度校准的组分化学平衡模型,对纯/非纯CO
2
-H
2
O体系的p H值进行了计算和预测评价。结果表明:N
2
和CH
4
均会对CO
2
饱和体系产生影响,使CO
2
在水中的溶解度降低,p H值增大,且CH
4
的影响大于N
2
。模型能较好地进行纯CO
2
-水体系的p H值预测,最大偏差不超过0.05个pH;在非纯CO
2
-H
2
O体系中有一定的偏差,主要为50℃以及CO
2
和杂质气体比例为1∶9的条件下,偏差在0.15个pH值以内。电势法和光谱法能进行高温高压条件下的原位pH值测量,纯/非纯CO
2
-H
2
O体系的pH预测模型具有较好的准确性,本文的研究成果为非纯CO
2
注入地层产生的化学变化提供了理论参考,对提高碳封存的安全性和有效性具有重要意义。
The dissolution of CO2-containing gases into deep aquifers results in the formation of carbonic acid
which lowers the pH value of the aquifer and may cause the dissolution or precipitation of minerals
thereby affecting the safety and effectiveness of CO2 geological utilization and storage. ObjectivepH is a key parameter for characterizing the chemical properties of a solution. Experimental measurement and model prediction of the pH values of pure and impure CO2-saturated systems can be used to evaluate the chemical changes under CO2 geological storage conditions. MethodsIn this study
the pH values of pure and impure CO2-water systems were measured in situ using potentiometric and spectroscopic methods
under temperatures conditions ranging from 35 to 93℃ and pressure condictions raging from 0.38 to 18 MPa. A component chemical equilibrium model calibrated using solubility data
was developed to calculate and predict the pH values of pure and impure CO2-water systems. ResultsThe results show that that N2 and CH4 influence the CO2-saturated systems by reducing CO2 solubility in water and increasing the pH value
with CH4 having a greater effect than N2. The model can accurately predict the pH values of pure CO2-water systems
with a maximum deviation within 0.05 pH units. In impure CO2-water systems
deviations are mainly observed under the condition of 50℃ and a CO2-to-impurity gas ratio of 1∶9
with deviations within 0.15 pH units. ConclusionThe potentiometric and spectroscopic methods are applicable for in situ pH measurements under high-temperature and high-pressure conditions
and the pH prediction model for pure and impure CO2-water systems shows good accuracy. The findings provide theoretical support for understanding the chemical changes induced by the injection of impure CO2 into geological formations
which is of great significance for enhancing the safety and effectiveness of carbon storage.
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