Characterization of the microbial activity impacts on transport and storage of hydrogen is a crucial aspect of successful Underground Hydrogen Storage (UHS). Microbes can use hydrogen for their metabolism, which can then lead to formation of biofilms. Biofilms can potentially alter the wettability of the system and, consequently, impact the flow dynamics and trapping mechanisms in the reservoir. In this study, we investigate the impact of microbial activity on wettability of the hydrogen/brine/rock system, using the captive-bubble cell experimental approach. Apparent contact angles are measured for bubbles of pure hydrogen in contact with a solid surface inside a cell filled with living brine which contains sulphate reducing microbes. To investigate the impact of surface roughness, two different solid samples are used: a "rough" Bentheimer Sandstone sample and a "smooth" pure Quartz sample. It is found that, in systems where buoyancy and interfacial forces are the main acting forces, the impact of biofilm formation on the apparent contact angle highly depends on the surface roughness. For the "rough" Bentheimer sandstone, the apparent contact angle was unchanged by biofilm formation, while for the smooth pure Quartz sample the apparent contact angle decreased significantly, making the system more water-wet. This decrease in apparent contact angle is in contrast with an earlier study present in the literature where a significant increase in contact angle due to microbial activity was reported. The wettability of the biofilm is mainly determined by the consistency of the Extracellular Polymeric Substances (EPS) which depends on the growth conditions in the system. Therefore, to determine the impact of microbial activity on the wettability during UHS will require accurate replication of the reservoir conditions including surface roughness, chemical composition of the brine, the microbial community, as well as temperature, pressure and pH-value conditions.

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To safely and efficiently utilize porous reservoirs for underground hydrogen storage (UHS), it is essential to characterize hydrogen transport properties at multiple scales. In this study, hydrogen/brine multiphase flow at 50 bar and 25 °C in a 17 cm Berea sandstone rock core was characterized and visualized at the pore and core scales using micro X-ray CT. The experiment included a single drainage and imbibition cycle during which relative permeability hysteresis was measured, and two no-flow periods to study the redistribution of hydrogen in the pore space during storage periods. An end-point relative permeability of 0.043 was found at Sw = 0.56, and the residual gas saturation was measured to be 0.32. Despite extensive pre-equilibration, significant dissolution of hydrogen into brine occurred near the core inlet due to elevated pressures and the corresponding increase in hydrogen solubility. During drainage, many disconnected hydrogen ganglia were observed further down the core which could be explained by the exsolution of the dissolved hydrogen. During imbibition, the dissolution of hydrogen led to the formation of preferential flow paths near the inlet, and eventually removed most of the trapped hydrogen in the final stage of the experiment. The two no-flow periods were characterized by the fragmentation of medium-sized hydrogen ganglia and the growth of a few larger ganglia, providing evidence for hydrogen re-connection through the dissolution-driven process of Ostwald ripening. These results demonstrate that despite the low solubility of hydrogen in brine, hydrogen dissolution can significantly influence the observed multiphase flow and trapping behavior in the reservoir and should be considered in UHS modeling.@en

To safely and efficiently utilize porous reservoirs for underground hydrogen storage (UHS), it is essential to characterize hydrogen transport properties at multiple scales. In this study, hydrogen/brine multiphase flow at 50 bar and 25 °C in a 17 cm Berea sandstone rock core was characterized and visualized at the pore and core scales using micro X-ray CT. The experiment included a single drainage and imbibition cycle during which relative permeability hysteresis was measured, and two no-flow periods to study the redistribution of hydrogen in the pore space during storage periods. An end-point relative permeability of 0.043 was found at Sw = 0.56, and the residual gas saturation was measured to be 0.32. Despite extensive pre-equilibration, significant dissolution of hydrogen into brine occurred near the core inlet due to elevated pressures and the corresponding increase in hydrogen solubility. During drainage, many disconnected hydrogen ganglia were observed further down the core which could be explained by the exsolution of the dissolved hydrogen. During imbibition, the dissolution of hydrogen led to the formation of preferential flow paths near the inlet, and eventually removed most of the trapped hydrogen in the final stage of the experiment. The two no-flow periods were characterized by the fragmentation of medium-sized hydrogen ganglia and the growth of a few larger ganglia, providing evidence for hydrogen re-connection through the dissolution-driven process of Ostwald ripening. These results demonstrate that despite the low solubility of hydrogen in brine, hydrogen dissolution can significantly influence the observed multiphase flow and trapping behavior in the reservoir and should be considered in UHS modeling.@en

Underground Hydrogen Storage (UHS) is an emerging large-scale energy storage technology. Researchers are investigating its feasibility and performance, including its injectivity, productivity, and storage capacity through numerical simulations. However, several ad-hoc relative permeability and capillary pressure functions have been used in the literature, with no direct link to the underlying physics of the hydrogen storage and production process. Recent relative permeability measurements for the hydrogen-brine system show very low hydrogen relative permeability and strong liquid phase hysteresis, very different to what has been observed for other fluid systems for the same rock type. This raises the concern as to what extend the existing studies in the literature are able to reliably quantify the feasibility of the potential storage projects. In this study, we investigate how experimentally measured hydrogen-brine relative permeability hysteresis affects the performance of UHS projects through numerical reservoir simulations. Relative permeability data measured during a hydrogen-water core-flooding experiment within ADMIRE project is used to design a relative permeability hysteresis model. Next, numerical simulation for a UHS project in a generic braided-fluvial water-gas reservoir is performed using this hysteresis model. A performance assessment is carried out for several UHS scenarios with different drainage relative permeability curves, hysteresis model coefficients, and injection/production rates. Our results show that both gas and liquid relative permeability hysteresis play an important role in UHS irrespective of injection/production rate. Ignoring gas hysteresis may cause up to 338% of uncertainty on cumulative hydrogen production, as it has negative effects on injectivity and productivity due to the resulting limited variation range of gas saturation and pressure during cyclic operations. In contrast, hysteresis in the liquid phase relative permeability resolves this issue to some extent by improving the displacement of the liquid phase. Finally, implementing relative permeability curves from other fluid systems during UHS performance assessment will cause uncertainty in terms of gas saturation and up to 141% underestimation on cumulative hydrogen production. These observations illustrate the importance of using relative permeability curves characteristic of hydrogen-brine system for assessing the UHS performances.

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Characterizing the wettability of hydrogen (H₂)–methane (CH₄) mixtures in subsurface reservoirs is the first step towards understanding containment and transport properties for underground hydrogen storage (UHS). In this study, we investigate the static contact angles of H₂–CH₄ mixtures, in contact with brine and Bentheimer sandstone rock using a captive-bubble cell device at different pressures, temperatures and brine salinity values. It is found that, under the studied conditions, H₂ and CH₄ show comparable wettability behaviour with contact angles ranging between [25°–45°]; and consequently their mixtures behave similar to the pure gas systems, independent of composition, pressure, temperature and salinity. For the system at rest, the acting buoyancy and surface forces allow for theoretical sensitivity analysis for the captive-bubble cell approach to characterize the wettability. Moreover, it is theoretically validated that under similar Bond numbers and similar bubble sizes, the contact angles of H₂ and CH₄ bubbles and their mixtures are indeed comparable. Consequently, in large-scale subsurface storage systems where buoyancy and capillary are the main acting forces, H₂, CH₄ and their mixtures will have similar wettability characteristics.

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Underground Hydrogen Storage (UHS) is an attractive technology for large-scale (TWh) renewable energy storage. To ensure the safety and efficiency of the UHS, it is crucial to quantify the H₂ interactions with the reservoir fluids and rocks across scales, including the micro scale. This paper reports the experimental measurements of advancing and receding contact angles for different channel widths for a H₂/water system at P = 10 bar and T = 20 °C using a microfluidic chip. To analyse the characteristics of the H₂ flow in straight pore throats, the network is designed such that it holds several straight channels. More specifically, the width of the microchannels range between 50 μm and 130 μm. For the drainage experiments, H₂ is injected into a fully water saturated system, while for the imbibition tests, water is injected into a fully H₂-saturated system. For both scenarios, high-resolution images are captured starting the introduction of the new phase into the system, allowing for fully-dynamic transport analyses. For better insights, N₂/water and CO₂/water flows were also analysed and compared with H₂/water. Results indicate strong water-wet conditions with H₂/water advancing and receding contact angles of, respectively, 13°–39°, and 6°–23°. It was found that the contact angles decrease with increasing channel widths. The receding contact angle measured in the 50 μm channel agrees well with the results presented in the literature by conducting a core-flood test for a sandstone rock. Furthermore, the N₂/water and CO₂/water systems showed similar characteristics as the H₂/water system. In addition to the important characterization of the dynamic wettability, the results are also crucially important for accurate construction of pore-scale simulators.

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Geological porous reservoirs provide the volume capacity needed for large scale underground hydrogen storage (UHS). To effectively exploit these reservoirs for UHS, it is crucial to characterize the hydrogen transport properties inside porous rocks. In this work, for the first time in the community, we have performed H ₂/water multiphase flow experiments at core scale under medical X-ray CT scanner. This has allowed us to directly image the complex transport properties of H ₂ when it is injected or retracted from the porous rock. The important effective functions of capillary pressure and relative permeability are also measured, for both drainage and imbibition. The capillary pressure measurements are combined with MICP data to derive a receding contact angle for the H ₂/water/sandstone rock system. The rock core sample is a heterogeneous Berea sandstone (17 cm long and 3.8 cm diameter). Our investigation reveals the interplay between gravitational, capillary, and viscous forces. More specifically, it illustrates complex displacement patterns in the rock, including gravity segregation, enhancement of spreading of H ₂ due to capillary barriers, and the formation of fingers/channel during imbibition which lead to significant trapping of hydrogen. These findings shed new light on our fundamental understanding of the transport characteristics of H ₂/water relevant for UHS.

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