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Dissolved silicate (H4SiO4) is essential for the formation of the opaline skeletal structures of diatoms and other siliceous plankton. A fraction of particulate biogenic silica (bSi) formed in surface waters sinks to the seabed, where it either dissolves and returns to the water column or is permanently buried. Global silica budgets are still poorly constrained since data on benthic bSi cycling are lacking, especially on continental margins. This study describes benthic bSi cycling in the Skagerrak, a sedimentary depocenter for particles from the North Sea. Biogenic silica burial fluxes, benthic H4SiO4 fluxes to the water column and bSi burial efficiencies are reported for nine stations by evaluating data from in-situ benthic landers and sediment cores with a diagenetic reaction-transport model. The model simulates bSi contents and H4SiO4 concentrations at all sites using a novel power law to describe bSi dissolution kinetics with a small number of adjustable parameters. Our results show that, on average, 1100 mmol m-2 yr-1 of bSi rains down to the Skagerrak basin seafloor, of which 50% is released back to overlying waters, with the remainder being buried. Biogenic silica cycling in the Skagerrak is generally consistent with previously reported global trends, showing higher Si fluxes and burial efficiencies than deep-sea sites and similar values compared to other continental margins. A significant finding of this work is a molar bSi-to-organic carbon burial ratio of 0.22 in Skagerrak sediments, which is distinctively lower compared to other continental margins. We suggest that the continuous dissolution of bSi in suspended sediments transported over long distances from the North Sea leads to the apparent decoupling between bSi and organic carbon in Skagerrak sediments.

Highlights • An artificial CO2 release demonstrated MMV techniques for offshore CCS. • Detection of leakage was demonstrated using acoustic, chemical and physical approaches. • Attribution of leakage was proved possible using artificial and natural tracer compounds. • Leakage quantification was possible using approaches not previously applied to CCS studies. • Non-catastrophic leaks were detected at levels below those that would cause environmental harm. Carbon capture and storage is a key mitigation strategy proposed for keeping the global temperature rise below 1.5 °C. Offshore storage can provide up to 13% of the global CO2 reduction required to achieve the Intergovernmental Panel on Climate Change goals. The public must be assured that potential leakages from storage reservoirs can be detected and that therefore the CO2 is safely contained. We conducted a controlled release of 675 kg CO2 within sediments at 120 m water depth, to simulate a leak and test novel detection, quantification and attribution approaches. We show that even at a very low release rate (6 kg day−1), CO2 can be detected within sediments and in the water column. Alongside detection we show the fluxes of both dissolved and gaseous CO2 can be quantified. The CO2 source was verified using natural and added tracers. The experiment demonstrates that existing technologies and techniques can detect, attribute and quantify any escape of CO2 from sub-seabed reservoirs as required for public assurance, regulatory oversight and emissions trading schemes.

The fluids emanating from active submarine hydrothermal vent chimneys provide a window into subseafloor processes and, through mixing with seawater, are responsible for steep thermal and compositional gradients that provide the energetic basis for diverse biological communities. Although several models have been developed to better understand the dynamic interplay of seawater, hydrothermal fluid, minerals and microorganisms inside chimney walls, none provide a fully integrated approach to quantifying the biogeochemistry of these hydrothermal systems. In an effort to remedy this, a fully coupled biogeochemical reaction-transport model of a hydrothermal vent chimney has been developed that explicitly quantifies the rates of microbial catalysis while taking into account geochemical processes such as fluid flow, solute transport and oxidation–reduction reactions associated with fluid mixing as a function of temperature. The metabolisms included in the reaction network are methanogenesis, aerobic oxidation of hydrogen, sulfide and methane and sulfate reduction by hydrogen and methane. Model results indicate that microbial catalysis is generally fastest in the hottest habitable portion of the vent chimney (77–102 °C), and methane and sulfide oxidation peak near the seawater-side of the chimney. The fastest metabolisms are aerobic oxidation of H2 and sulfide and reduction of sulfate by H2 with maximum rates of 140, 900 and 800 pmol cm−3 d−1, respectively. The maximum rate of hydrogenotrophic methanogenesis is just under 0.03 pmol cm−3 d−1, the slowest of the metabolisms considered. Due to thermodynamic inhibition, there is no anaerobic oxidation of methane by sulfate (AOM). These simulations are consistent with vent chimney metabolic activity inferred from phylogenetic data reported in the literature. The model developed here provides a quantitative approach to describing the rates of biogeochemical transformations in hydrothermal systems and can be used to constrain the role of microbial activity in the deep subsurface.