SUPERCRITICAL CO2
; CARBON-DIOXIDE
; REACTIVITY
; KINETICS
; WATER
; DISSOLUTION
; SORPTION
; CLAYS
; SHALE
WOS学科分类:
Engineering, Chemical
WOS研究方向:
Engineering
英文摘要:
One of the challenges of the present century is to limit the greenhouse gas emissions for the mitigation of climate change which is possible for example by a transitional technology, CO2 geological storage. Clay minerals are considered to be responsible for the low permeability and sealing capacity of caprocks sealing off stored CO2. However, their reactions are not well understood for complex simulations. This work aims to create a kinetic geochemical model of Na-montmorillonite standard SWy-2 supported by solution and mineral composition results from batch experiments. Such experimentally validated numerical models are scarce. Four 70-hours experiments have been carried out at atmospheric conditions, and with CO2 supercritical phase at 100 bar and 80 degrees C. Solution samples have been taken during and after experiments and their compositions were measured by ICP-OES. The treated solid phase has been analyzed by XRD and ATR-FTIR and compared to in-parallel measured references (dried SWy-2). Kinetic geochemical modelling of the experimental conditions has been performed by software PHREEQC. Experiments and models show fast reactions under the studied conditions and increased reactivity in presence of scCO(2). Solution composition results cannot be described by the change of the uncertain reactive surface area of mineral phases. By considering the clay standard's cation exchange capacity divided proportionally among interlayer cations of Na-montmorillonite, the measured variation can be described on an order of magnitude level. It is furthermore indicated that not only the interlayer cations take part in this process but a minor proportion of other, structural ions as well, differently in the reference and scCO(2) environments.
1.Eotvos Lorand Univ, Fac Sci, Inst Geog & Earth Sci, Lithosphere Fluid Res Lab,Dept Petrol & Geochem, Pazmany Peter Setany 1-C, H-1117 Budapest, Hungary 2.Hungarian Acad Sci, MTA Premium Postdoctoral Res Program, MTA Off Res Grp Attached Univ & Other Inst, Nador U 7, H-1051 Budapest, Hungary 3.Budapest Univ Technol & Econ, Fac Chem Technol & Biotechnol, Dept Chem & Environm Proc Engn, Muegyet Rakpart 3, H-1111 Budapest, Hungary 4.Cement Ind Ltd, CEMKUT Res & Dev, Becsi Ut 122-124, H-1034 Budapest, Hungary 5.KTI Inst Transport Sci Nonprofit Ltd, Than Karoly U 3-S, H-1119 Budapest, Hungary 6.Min & Geol Surveyof Hungary, Dept Hydrogeol & Geochem, Stefania Ut 14, H-1143 Budapest, Hungary 7.Hungarian Acad Sci, Res Ctr Astron & Earth Sci, Geog Inst, Budaorsi Ut 45, H-1112 Budapest, Hungary
Recommended Citation:
Szabo, Zsuzsanna,Hegyfalvi, Csaba,Freiler-Nagy, Agnes,et al. Geochemical Reactions of Na-montmorillonite in Dissolved scCO(2) in Relevance of Modeling Caprock Behavior in CO2 Geological Storage[J]. PERIODICA POLYTECHNICA-CHEMICAL ENGINEERING,2019-01-01,63(2):318-327