Pore-scale observations of CO2 thermodynamic properties and dissolution trapping in porous media

IF 5.9 1区 地球科学 Q1 ENGINEERING, CIVIL
Shaohua Li, Xin Wang, Lanlan Jiang, Yongchen Song
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Abstract

Carbon geological storage (CGS) presents a promising approach to mitigate climate change. Partially free CO2 is trapped in tiny pores and gradually dissolves into formation fluid. However, thermodynamic properties of CO2 remain inadequately understood, which strongly influence activation possibility of these free CO2. In this study, we innovatively mapped CO2 evolution and redistribution at micro scale by using X-ray CT. CO2 growth or shrinkage was determined by the threshold equal to pore volume. Bellow the threshold, bubbles experienced thermodynamically unstable shrink, following a power-law distribution in its specific interfacial area. Otherwise, bubble growth was governed by diffusion between gas and liquid phases, unlike conversely bubble coalescence. Larger bubbles expand at the expense of smaller ones through Ostwald ripening. The surface energy of CO2 bubbles during Ostwald ripening in porous media was firstly quantified. The whole system tended to reduce surface energy and larger bubbles have lower surface energy. In additional, high curvature interfaces prefer to rupture and growth. It was also found that CO2 bubble disappears in about 5.87 h at laboratory scales, which was 23.79 times greater than that estimated by the traditional LSW equation. This longer period allowed CO2 to redistribute within porous media, diminishing solubility and mineral trapping efficiency, thereby increasing the risk of long-term storage leakage.

Abstract Image

碳地质封存(CGS)是减缓气候变化的一种可行方法。部分游离的二氧化碳被困在微小的孔隙中,并逐渐溶解到地层流体中。然而,人们对二氧化碳的热力学特性仍缺乏足够的了解,而这些特性对这些游离二氧化碳的活化可能性有很大影响。在这项研究中,我们利用 X 射线 CT 创新性地绘制了二氧化碳在微观尺度上的演化和再分布图。二氧化碳的增长或收缩是由与孔隙体积相等的阈值决定的。在阈值以下,气泡会出现热力学上不稳定的收缩,其比界面面积呈幂律分布。否则,气泡的增长受气相和液相之间的扩散控制,而气泡的凝聚则不同。通过奥斯特瓦尔德熟化作用,较大气泡的膨胀以较小气泡的膨胀为代价。首先对多孔介质中奥斯特瓦尔德熟化过程中二氧化碳气泡的表面能进行了量化。整个系统趋于降低表面能,较大的气泡表面能较低。此外,高曲率界面更倾向于破裂和生长。研究还发现,在实验室尺度上,二氧化碳气泡消失的时间约为 5.87 小时,是传统 LSW 方程估计时间的 23.79 倍。更长的时间使得二氧化碳在多孔介质中重新分布,降低了溶解度和矿物捕集效率,从而增加了长期封存泄漏的风险。
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来源期刊
Journal of Hydrology
Journal of Hydrology 地学-地球科学综合
CiteScore
11.00
自引率
12.50%
发文量
1309
审稿时长
7.5 months
期刊介绍: The Journal of Hydrology publishes original research papers and comprehensive reviews in all the subfields of the hydrological sciences including water based management and policy issues that impact on economics and society. These comprise, but are not limited to the physical, chemical, biogeochemical, stochastic and systems aspects of surface and groundwater hydrology, hydrometeorology and hydrogeology. Relevant topics incorporating the insights and methodologies of disciplines such as climatology, water resource systems, hydraulics, agrohydrology, geomorphology, soil science, instrumentation and remote sensing, civil and environmental engineering are included. Social science perspectives on hydrological problems such as resource and ecological economics, environmental sociology, psychology and behavioural science, management and policy analysis are also invited. Multi-and interdisciplinary analyses of hydrological problems are within scope. The science published in the Journal of Hydrology is relevant to catchment scales rather than exclusively to a local scale or site.
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