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Abstract We investigated the effect of an artificial CO2 vent (0.0015−0.037 mol s−1), simulating a leak from a reservoir for carbon capture and storage (CCS), on the sediment geochemistry. CO2 was injected 3 m deep into the seafloor at 120 m depth. With increasing mass flow an increasing number of vents were observed, distributed over an area of approximately 3 m. In situ profiling with microsensors for pH, T, O2 and ORP showed the geochemical effects are localized in a small area around the vents and highly variable. In measurements remote from the vent, the pH reached a value of 7.6 at a depth of 0.06 m. In a CO2 venting channel, pH reduced to below 5. Steep temperature profiles were indicative of a heat source inside the sediment. Elevated total alkalinity and Ca2+ levels showed calcite dissolution. Venting decreased sulfate reduction rates, but not aerobic respiration. A transport-reaction model confirmed that a large fraction of the injected CO2 is transported laterally into the sediment and that the reactions between CO2 and sediment generate enough heat to elevate the temperature significantly. A CO2 leak will have only local consequences for sediment biogeochemistry, and only a small fraction of the escaped CO2 will reach the sediment surface.

This work is focused on results from a recent controlled sub-seabed in situ carbon dioxide (CO2) release experiment carried out during May–October 2012 in Ardmucknish Bay on the Scottish west coast. Three types of pCO2 sensors (fluorescence, NDIR and ISFET-based technologies) were used in combination with multiparameter instruments measuring oxygen, temperature, salinity and currents in the water column at the epicentre of release and further away. It was shown that distribution of seafloor CO2 emissions features high spatial and temporal heterogeneity. The highest pCO2 values (∼1250 μatm) were detected at low tide around a bubble stream and within centimetres distance from the seafloor. Further up in the water column, 30–100 cm above the seabed, the gradients decreased, but continued to indicate elevated pCO2 at the epicentre of release throughout the injection campaign with the peak values between 400 and 740 μatm. High-frequency parallel measurements from two instruments placed within 1 m from each other, relocation of one of the instruments at the release site and 2D horizontal mapping of the release and control sites confirmed a localized impact from CO2 emissions. Observed effects on the water column were temporary and post-injection recovery took <7 days. A multivariate statistical approach was used to recognize the periods when the system was dominated by natural forcing with strong correlation between variation in pCO2 and O2, and when it was influenced by purposefully released CO2. Use of a hydrodynamic circulation model, calibrated with in situ data, was crucial to establishing background conditions in this complex and dynamic shallow water system.

In this work, the wastewater obtained from the hydrothermal liquefaction of black liquor was treated and valorized for hydrogen production by supercritical water gasification (SCWG). The influence of the main process parameters on the conversion yield was studied. The experiments were conducted at three different temperatures (below and above the critical point of water): 350 °C, 450 °C and 600 °C. The results showed that by increasing the temperature from 350 °C to 600 °C, the total gas yield was highly improved (from 1.9 mol gas/kg of dried feedstock to 13.1 mol gas/kg of dried feedstock). The H2 composition was higher than that of CH4 and CO2 at 600 °C, and the HHV of the obtained gas was 61.2 MJ/kg. The total organic carbon (TOC) removal efficiency was also improved by increasing the temperature, indicating that the SCWG process could be used for both applications: (i) for wastewater treatment; (ii) for producing a high calorific gas. The experiments with the Raney-nickel catalyst were performed in order to study the catalyst’s influence on the conversion yield. The results indicated that the catalyst enhances carbon conversion and gas production from mild to higher temperatures. The maximum total gas yield obtained with this catalyst was 32.4 mol gas/kg of dried feedstock at 600 °C, which is 2.5 times higher than that obtained at the same operating conditions without a catalyst. The H2 yield and the HHV of the obtained gas with the catalyst were 20.98 mol gas/kg dried feedstock and 80.2 MJ/kg, respectively. However, the major contribution of the catalytic SCWG process was the improvement of the total gas yield at mild operating temperatures (450 °C), and the obtained performance was even higher than that obtained at 600 °C without catalyst (17.81 mol gas/kg dried feedstock and 13.1 mol gas/kg dried feedstock, respectively). This is a sustainable approach for treating wastewater at mild temperatures by catalytic SCWG.

Abstract Sub-seabed geological CO2 storage is discussed as a climate mitigation strategy, but the impact of any leakage of stored CO2 into the marine environment is not well known. In this study, leakage from a CO2 storage reservoir through near-surface sediments was mimicked for low leakage rates in the North Sea. Field data were combined with laboratory experiments and transport-reaction modelling to estimate CO2 and mineral dissolution rates, and to assess the mobilization of metals in contact with CO2-rich fluids and their potential impact on the environment. We found that carbonate and silicate minerals reacted quickly with the dissolved CO2, increasing porewater alkalinity and neutralizing about 5% of the injected CO2. The release of Ca, Sr, Ba and Mn was mainly controlled by carbonate dissolution, while Fe, Li, B, Mg, and Si were released from silicate minerals, mainly from deeper sediment layers. No toxic metals were released from the sediments and overall the injected CO2 was only detected up to 1 m away from seabed CO2 bubble streams. Our results suggest that low leakage rates of CO2 over short timescales have minimal impact on the benthic environment. However, porewater composition and temperature are effective indicators for leakage detection, even at low CO2 leakage rates.

AbstractThe potential for leakage of CO2 from a storage reservoir into the overlying marine sediments and into the water column and the impacts on benthic ecosystems are major challenges associated with carbon capture and storage (CCS) in subseafloor reservoirs. We have conducted a field-scale controlled CO2 release experiment in shallow, unconsolidated marine sediments, and documented the changes to the chemical composition of the sediments, their pore waters and overlying water column before, during and up to 1 year after the 37-day long CO2 release. Increased levels of dissolved inorganic carbon (DIC) were detected in the pore waters close to the sediment-seawater interface in sediments sampled closest to the subsurface injection point within 5 weeks of the start of the CO2 release. Highest DIC concentrations (28.8mmolL−1, compared to background levels of 2.4mmolL−1) were observed 6 days after the injection had stopped. The high DIC pore waters have high total alkalinity, and low δ13CDIC values (−20‰, compared to a background value of −2‰), due to the dissolution of the injected CO2 (δ13C=−26.6‰). The high DIC pore waters have enhanced concentrations of metals (including Ca, Fe, Mn) and dissolved silicon, relative to non-DIC enriched pore waters, indicating that dissolution of injected CO2 promotes dissolution of carbonate and silicate minerals. However, in this experiment, the pore water metal concentrations did not exceed levels considered to be harmful to the environment. The spatial extent of the impact of the injected CO2 in the sediments and pore waters was restricted to an area within 25m of the injection point, and no impact was observed in the overlying water column. Concentrations of all pore water constituents returned to background values within 18 days after the CO2 injection was stopped.

This paper reviews research into the potential environmental impacts of leakage from geological storage of CO2 since the publication of the IPCC Special Report on Carbon Dioxide Capture and Storage in 2005. Possible impacts are considered on onshore (including drinking water aquifers) and offshore ecosystems. The review does not consider direct impacts on man or other land animals from elevated atmospheric CO2 levels. Improvements in our understanding of the potential impacts have come directly from CO2 storage research but have also benefitted from studies of ocean acidification and other impacts on aquifers and onshore near surface ecosystems. Research has included observations at natural CO2 sites, laboratory and field experiments and modelling. Studies to date suggest that the impacts from many lower level fault- or well-related leakage scenarios are likely to be limited spatially and temporarily and recovery may be rapid. The effects are often ameliorated by mixing and dispersion of the leakage and by buffering and other reactions; potentially harmful elements have rarely breached drinking water guidelines. Larger releases, with potentially higher impact, would be possible from open wells or major pipeline leaks but these are of lower probability and should be easier and quicker to detect and remediate.