title: Pore-scale study of transverse mixing induced CaCO₃ precipitation and permeability reduction in a model subsurface sedimentary system.
abstract: A microfluidic pore structure etched into a silicon wafer was used as a two-dimensional model subsurface sedimentary system (i.e., micromodel) to study mineral precipitation and permeability reduction relevant to groundwater remediation and geological carbon sequestration. Solutions containing CaCl(2) and Na(2)CO(3) at four different saturation states (Ω = [Ca(2+)][CO(3)(2-)]/K(spCaCO(3))) were introduced through two separate inlets, and they mixed by diffusion transverse to the main flow direction along the center of the micromodel resulting in CaCO(3) precipitation. Precipitation rates increased and the total amount of precipitates decreased with increasing saturation state, and only vaterite and calcite crystals were formed (no aragonite). The relative amount of vaterite increased from 80% at the lowest saturation state (Ω(v) = 2.8 for vaterite) to 95% at the highest saturation state (Ω(v) = 4.5). Fluorescent tracer tests conducted before and after CaCO(3) precipitation indicate that pore spaces were occluded by CaCO(3) precipitates along the transverse mixing zone, thus substantially reducing porosity and permeability, and potentially limiting transformation from vaterite to the more stable calcite. The results suggest that mineral precipitation along plume margins can decrease both reactant mixing during groundwater remediation, and injection and storage efficiency during CO(2) sequestration.
authors.affiliation: Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, USA.
authors.forename: Changyong
authors.initials: C
authors.lastname: Zhang
authors.forename: Karl
authors.initials: K
authors.lastname: Dehoff
authors.forename: Nancy
authors.initials: N
authors.lastname: Hess
authors.forename: Mart
authors.initials: M
authors.lastname: Oostrom
authors.forename: Thomas W
authors.initials: TW
authors.lastname: Wietsma
authors.forename: Albert J
authors.initials: AJ
authors.lastname: Valocchi
authors.forename: Bruce W
authors.initials: BW
authors.lastname: Fouke
authors.forename: Charles J
authors.initials: CJ
authors.lastname: Werth
mesh_terms: D002119:Calcium Carbonate / Q000737:chemistry*; D019015:Geologic Sediments / Q000737:chemistry*; D008853:Microscopy; D008962:Models, Theoretical; D010539:Permeability; D013059:Spectrum Analysis, Raman
chemical_list: D002119:Calcium Carbonate