CO 2 injection Laboratory experiments and modeling Josep M Soler Lídia FernándezRojo Ignasi Queralt Jordi Cama IDAEACSIC Catalonia Spain M Carme Chaparro ID: 1021433
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1. Flow and reaction along the cement-rock interface during CO2 injection. Laboratory experiments and modeling.Josep M. Soler, Lídia Fernández-Rojo, Ignasi Queralt, Jordi CamaIDAEA-CSIC, Catalonia, SpainM. Carme ChaparroKIT-INE, GermanySalvador GalíUniv. de Barcelona, Catalonia, SpainEGU2020, May 5th, 20201
2. 2CO2 storage
3. 3RockCementCasingCO2BoreholePotential leakage alongcement-rock interface
4. 4Laboratory experimentsInjection of synthetic groundwaterSynthetic groundwater, 70 – 72 daysCl Na Ca SO4 Mg, I 0.6, pH 6.210-3.4 bar PCO2, 25C.Synthetic groundwater, 15 – 20 daysCl Na Ca SO4 Mg, I 0.6, pH 3.2130 bar PCO2, 60CRockCementChannel
5. 5Inputsynthetic saline solution (M)Ca2+ 0.050SO42- 0.027Mg2+ 0.032K+ 0.011Na+ 0.390Cl- 0.500Br- 0.011Atmospheric CO2 reactorSupercritical CO2 reactorTemperature = 60 ºCP = 130 bar CO2 pH ~ 3.0Q = 0.05 mL/minResidence time ~4 minSolid sampleTemperature = 25 ºCP = 10-3.4 bar CO2 pH ~ 6.2Q = 0.05 mL/minResidence time ~2.5 min
6. 6Inputsynthetic saline solution (M)Ca2+ 0.050SO42- 0.027Mg2+ 0.032K+ 0.011Na+ 0.390Cl- 0.500Br- 0.011Atmospheric CO2 reactorSupercritical CO2 reactorTemperature = 60 ºCP = 130 bar CO2 pH ~ 3.0Q = 0.05 mL/minResidence time ~4 minSolid sampleTemperature = 25 ºCP = 10-3.4 bar CO2 pH ~ 6.2Q = 0.05 mL/minResidence time ~2.5 minreactorreactor
7. 7Cement – limestone/sandstone/marl (all rocks with high calcite contents)(1) LiBr pulse tracer test (atm-CO2 experiments) to determine Deff for cement. Rock porosities (ca. 5%) and Deff (10-13 m2/s range) are smaller (previous studies).(2) Injection of synthetic groundwater (atm-CO2 and supc-CO2 experiments).Laboratory experiments
8. 8SEM post mortemGypsum precipitation
9. 9Profilometry (supc-CO2)mm
10. 10InletInletOutletOutletRockCementPicture – limestone experiment (supc-CO2)
11. 112D reactive transport modeling (CrunchFlow)Flow channel: advection + dispersionCement, rock: diffusion
12. 12LiBr pulse tracer test (atm-CO2 experiments) Fitting of Deff for cement
13. 13(2) Injection of synthetic groundwater Fitting of reactive surface areasRock - primary phasesThermodynamicdataKineticdataCement phases Secondary phasesbrucite, gypsum, jarosite, aluniteCEMDATA14EQ3/6EQ3/6Fast kinetics, leading to local equilibriumFrom literatureFast kinetics, leading to local equilibrium
14. 14LimestoneSandstoneMarlOutlet solutionpHDCa (mol/kgw)
15. 15LimestoneSandstoneMarlOutlet solutionpHDCa (mol/kgw)Tracer testStart of Mg(OH)2 precipitationClosing of cementporosity
16. 16LimestoneSandstoneMarlOutlet solutionDMg (mol/kgw)DS (mol/kgw)
17. 17Model:Mineralvolumefractionsatm-CO2supc-CO2LimestoneSandstoneMarl
18. 18Model:MineralvolumefractionsCa(OH)2 dissltn.Mg(OH)2 pptn, gypsum pptn.Mg, SO4 from groundwateratm-CO2supc-CO2LimestoneSandstoneMarl
19. 19Portlandite dissltn (ettringite, Si-hydrogarnet, hydrotalcite) dissltnCalcite, (gypsum) pptnCalcite dissltn - (Gypsum pptn)Reaction fronts:supc-CO2
20. 20Model: Porosities
21. 21ConclusionsCement alteration much stronger than rock alteration (larger reactivities and Deff).Closing of cement porosity next to flow channel under atmospheric conditions (brucite precipitation), but opening of porosity under supercritical conditions. Implemented reactive surface areas for portlandite, ettringite and Si-hydrogarnet (cement) under atmospheric conditions had to be smaller than under supercritical conditions (2 to 4 orders of magnitude).Effect of P on gypsum solubility had to be implemented for supercritical conditions(phreeqc v3).Calculated small amounts of ferrihydrite, gibbsite and boehmite could partially contributeto the amorphous reddish precipitates observed on the rock (supc-CO2). Additional amorphous phases are probably involved.
22. 22AcknowledgementsThis study was financed by projects CGL2017-82331-R (Spanish Ministry of Economy and Competitiveness), with contribution of FEDER funds, CEX2018-000794-S (Spanish Ministry of Science and Innovation) and 2017SGR 1733 (Catalan Government). We would like to thank Ramón Vázquez for the design and construction of the supercritical CO2 reactor as well as all the technical staff that has participated in chemical and mineralogical analyses: Jordi Bellés, Maite Romero, Bàrbara Baena, Javier García, David Artiaga, Josep Bassas, Jordi Díaz, Aránzazu Villuendas and Natalia Moreno.