This article identifies and discusses the scientific challenges of hydrogen storage in porous media for safe and efficient large-scale energy storage to enable a global hydrogen economy.

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The geological storage of hydrogen is necessary to enable the successful transition to a hydrogen economy and achieve net-zero emissions targets. Comprehensive investigations must be undertaken for each storage site to ensure their long-term suitability and functionality. As such, the systematic infrastructure and potential risks of large-scale hydrogen storage must be established. Herein, we conducted over 250 batch reaction experiments with different types of reservoir sandstones under conditions representative of the subsurface, reflecting expected time scales for geological hydrogen storage, to investigate potential reactions involving hydrogen. Each hydrogen experiment was paired with a hydrogen-free control under otherwise identical conditions to ensure that any observed reactions were due to the presence of hydrogen. The results conclusively reveal that there is no risk of hydrogen loss or reservoir integrity degradation due to abiotic geochemical reactions in sandstone reservoirs.

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Abstract. Dissolved inorganic carbon (DIC) fluxes across the vadose zone are influenced by a complex interplay of biological, chemical and physical factors. A novel soil mesocosm system was evaluated as a tool for providing information on the mechanisms behind DIC percolation to the groundwater from unplanted soil. Carbon dioxide partial pressure (pCO2), alkalinity, soil moisture and temperature were measured with depth and time, and DIC in the percolate was quantified using a sodium hydroxide trap. Results showed good reproducibility between two replicate mesocosms. The pCO2 varied between 0.2 and 1.1%, and the alkalinity was 0.1–0.6 meq L−1. The measured cumulative effluent DIC flux over the 78-day experimental period was 185–196 mg L−1 m−2 and in the same range as estimates derived from pCO2 and alkalinity in samples extracted from the side of the mesocosm column and the drainage flux. Our results indicate that the mesocosm system is a promising tool for studying DIC percolation fluxes and other biogeochemical transport processes in unsaturated environments.

Abstract. The efflux of carbon dioxide (CO2) from soils influences atmospheric CO2 concentrations and thereby climate change. The partitioning of inorganic carbon (C) fluxes in the vadose zone between emission to the atmosphere and to the groundwater was investigated to reveal controlling underlying mechanisms. Carbon dioxide partial pressure in the soil gas (pCO2), alkalinity, soil moisture and temperature were measured over depth and time in unplanted and planted (barley) mesocosms. The dissolved inorganic carbon (DIC) percolation flux was calculated from the pCO2, alkalinity and the water flux at the mesocosm bottom. Carbon dioxide exchange between the soil surface and the atmosphere was measured at regular intervals. The soil diffusivity was determined from soil radon-222 (222Rn) emanation rates and soil air Rn concentration profiles and was used in conjunction with measured pCO2 gradients to calculate the soil CO2 production. Carbon dioxide fluxes were modeled using the HP1 module of the Hydrus 1-D software. The average CO2 effluxes to the atmosphere from unplanted and planted mesocosm ecosystems during 78 days of experiment were 0.1 ± 0.07 and 4.9 ± 0.07 μmol C m−2 s−1, respectively, and grossly exceeded the corresponding DIC percolation fluxes of 0.01 ± 0.004 and 0.06 ± 0.03 μmol C m−2 s−1. Plant biomass was high in the mesocosms as compared to a standard field situation. Post-harvest soil respiration (Rs) was only 10% of the Rs during plant growth, while the post-harvest DIC percolation flux was more than one-third of the flux during growth. The Rs was controlled by production and diffusivity of CO2 in the soil. The DIC percolation flux was largely controlled by the pCO2 and the drainage flux due to low solution pH. Modeling suggested that increasing soil alkalinity during plant growth was due to nutrient buffering during root nitrate uptake.

Abstract. The efflux of carbon dioxide (CO2) from soils influences atmospheric CO2 concentrations and thereby climate change. The partitioning of inorganic carbon fluxes in the vadose zone between emission to the atmosphere and to the groundwater was investigated. Carbon dioxide partial pressure in the soil gas (pCO2), alkalinity, soil moisture and temperature were measured over depth and time in unplanted and planted (barley) mesocosms. The dissolved inorganic carbon (DIC) percolation flux was calculated from the pCO2, alkalinity and the water flux at the mesocosm bottom. Carbon dioxide exchange between the soil surface and the atmosphere was measured at regular intervals. The soil diffusivity was determined from soil radon-222 (222Rn) emanation rates and soil air Rn concentration profiles, and was used in conjunction with measured pCO2 gradients to calculate the soil CO2 production. Carbon dioxide fluxes were modelled using the HP1 module of the Hydrus 1-D software. The average CO2 effluxes to the atmosphere from unplanted and planted mesocosm ecosystems during 78 days of experiment were 0.1 ± 0.07 and 4.9 ± 0.07 μmol carbon (C) m−2 s−1, respectively, and largely exceeded the corresponding DIC percolation fluxes of 0.01 ± 0.004 and 0.06 ± 0.03 μmol C m−2 s−1. Post-harvest soil respiration (Rs) was only 10% of the Rs during plant growth, while the post-harvest DIC percolation flux was more than one third of the flux during growth. The Rs was controlled by production and diffusivity of CO2 in the soil. The DIC percolation flux was largely controlled by the pCO2 and the drainage flux due to low solution pH. Plant biomass and soil pCO2 were high in the mesocosms as compared to a standard field situation. Our results indicate no change of the cropland C balance under elevated atmospheric CO2 in a warmer future climate, in which plant biomass and soil pCO2 are expected to increase.

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