Injection and subsequent carbonation of calcium and magnesium silicate particles are proposed here as a novel strategy to grout fractures or pores and decrease fluid conductivity in the deep subsurface by taking advantage of favorable reaction kinetics. This approach could be used to manage legacy environmental risks from energy extraction techniques such as hydraulic fracturing of shale formations. To evaluate this approach, we studied the carbonation of wollastonite (CaSiO3) in the presence of ground shale under temperature and pressure (T/P) conditions broadly representative of the gas-producing regions of the Marcellus formation in the eastern United States. Effect of calcite (CaCO3) precipitation on shale particle morphology and interparticle pore structures was investigated and impacts on permeability were evaluated using batch and column experiments. Formation T/P were positively correlated with extent of carbonation. Side reactions involving calcium ions and passivation by amorphous silica did not appreciably impede the carbonation reaction. Quantitative X-ray diffraction results showed conversions in excess of 50% after 24 h, indicating that many shale plays possess the necessary T/P conditions for favorable carbonation kinetics. Scanning electron microscope–energy dispersive X-ray results showed that CaCO3 precipitates effectively cemented unconsolidated shale particles. Mercury intrusion results indicated that the porosity of column reactors packed with shale particles decreased appreciably after reaction with CaSiO3 and CO2-saturated water. These CO2-mediated dissolution/precipitation reactions could form the basis of permeability control technologies to manage emerging risks of fluid leakage and contaminant migration from energy production and waste disposal activities in the deep subsurface.
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