Experimental investigation of hydrogen-carbonate reactions via computerized tomography: Implications for underground hydrogen storage

The underground hydrogen storage (UHS) in depleted hydrocarbon reservoirs, aquifers, and saline caverns is regarded as a vital component of hydrogen economy value-chains, meant to tackle carbon emissions and global warming. The caprock integrity and storage capacity of the carbonate formations can be altered by the reaction between the injected hydrogen and the calcite/dolomite minerals during UHS. However, experimental investigations of hydrogen-calcite/dolomite reactions at underground storage temperature are rarely reported in literature. Thus, we conducted X-ray computed micro-tomography (μCT) scans of limestone and dolomite cores before and after pressurization with hydrogen for 75 days at 700 psi and 75 °C. For the first time, a significant calcite expansion was observed and led to reduction in storage capacity (i.e., effective porosity) by 47%. However, the storage capacity of the dolomite rock slightly increased (～6%) because the grain expansion effects canceled out the dissolution effects. The study suggests that reduction in storage capacity of carbonate formation due to hydrogen reactivity with calcite is possible during UHS in carbonate formations. Thus, hydrogen reactivity with carbonate minerals should be evaluated to de-risk hydrogen storage projects in carbonate formations.