ALBERT

Description: Basalt weathering is one of many relevant processes balancing the global carbon cycle via land-ocean alkalinity fluxes. The CO2 consumption by weathering can be calculated using alkalinity and is often scaled with runoff and/or temperature. Here it is tested if information on the surface age distribution of a volcanic system is a useful proxy for changes in alkalinity production with time. A linear relationship between temperature normalized alkalinity fluxes and the Holocene area fraction of a volcanic field was identified, using information from 33 basalt volcanic fields, with an r2=0.91. This relationship is interpreted as an aging function and suggests that fluxes from Holocene areas are ~10 times higher than those from old inactive volcanic fields. However, the cause for the decrease with time is probably a combination of effects, including a decrease in alkalinity production from surface near material in the critical zone as well as a decline in hydrothermal activity and magmatic CO2 contribution. A comparison with global models suggests, that global alkalinity fluxes considering Holocene active basalt areas are ~70% higher than the average from these models imply. The contribution of Holocene areas to the global basalt alkalinity fluxes is however only ~6%, because identified, mapped Holocene basalt areas cover only ~1% of the existing basalt areas. The large trap basalt proportion on the global basalt areas today reduces the relevance of the aging effect. However, the aging effect might be a relevant process during periods of globally, intensive volcanic activity, which remains to be tested.

Description: Basalt weathering is one of many relevant processes balancing the global carbon cycle via land–ocean alkalinity fluxes. The CO2 consumption by weathering can be calculated using alkalinity and is often scaled with runoff and/or temperature. Here, it is tested if the surface age distribution of a volcanic system derived by geological maps is a useful proxy for changes in alkalinity production with time. A linear relationship between temperature normalized alkalinity fluxes and the Holocene area fraction of a volcanic field was identified using information from 33 basalt volcanic fields, with an r2=0.93. This relationship is interpreted as an aging function and suggests that fluxes from Holocene areas are ∼10 times higher than those from old inactive volcanic fields. However, the cause for the decrease with time is probably a combination of effects, including a decrease in alkalinity production from material in the shallow critical zone as well as a decline in hydrothermal activity and magmatic CO2 contribution. The addition of fresh reactive material on top of the critical zone has an effect in young active volcanic settings which should be accounted for, too. A comparison with global models suggests that global alkalinity fluxes considering Holocene basalt areas are ∼60 % higher than the average from these models imply. The contribution of Holocene areas to the global basalt alkalinity fluxes is today however only ∼5 %, because identified, mapped Holocene basalt areas cover only ∼1 % of the existing basalt areas. The large trap basalt proportion on the global basalt areas today reduces the relevance of the aging effect. However, the aging effect might be a relevant process during periods of globally intensive volcanic activity, which remains to be tested.

Description: Rivers are a major source of nutrients, carbon and alkalinity to the global ocean. In this study, we firstly estimate pre-industrial riverine loads of nutrients, carbon and alkalinity based on a hierarchy of weathering and terrestrial organic matter export models, while identifying regional hotspots of the riverine exports. Secondly, we implement the riverine loads into a global ocean biogeochemical model to describe their implications for oceanic nutrient concentrations, net primary production (NPP) and air–sea CO2 fluxes globally, as well as in an analysis of coastal regions. Thirdly, we quantitatively assess the terrestrial origins and the long-term fate of riverine carbon in the ocean. We quantify annual bioavailable pre-industrial riverine loads of 3.7 Tg P, 27 Tg N, 158 Tg Si and 603 Tg C delivered to the ocean globally. We thereby identify the tropical Atlantic catchments (20 % of global C), Arctic rivers (9 % of global C) and Southeast Asian rivers (15 % of global C) as dominant suppliers of carbon for the ocean. The riverine exports lead to a simulated net global oceanic CO2 source of 231 Tg C yr−1 to the atmosphere, which is mainly caused by inorganic carbon (source of 183 Tg C yr−1) and by organic carbon (source of 128 Tg C yr−1) riverine loads. Additionally, a sink of 80 Tg C yr−1 is caused by the enhancement of the biological carbon uptake from dissolved inorganic nutrient inputs from rivers and the resulting alkalinity production. While large outgassing fluxes are simulated mostly in proximity to major river mouths, substantial outgassing fluxes can be found further offshore, most prominently in the tropical Atlantic. Furthermore, we find evidence for the interhemispheric transfer of carbon in the model; we detect a larger relative outgassing flux (49 % of global riverine-induced outgassing) in the Southern Hemisphere in comparison to the hemisphere's relative riverine inputs (33 % of global C inputs), as well as an outgassing flux of 17 Tg C yr−1 in the Southern Ocean. The addition of riverine loads in the model leads to a strong NPP increase in the tropical west Atlantic, Bay of Bengal and the East China Sea (+166 %, +377 % and +71 %, respectively). On the light-limited Arctic shelves, the NPP is not strongly sensitive to riverine loads, but the CO2 flux is strongly altered regionally due to substantial dissolved inorganic and organic carbon supplies to the region. While our study confirms that the ocean circulation remains the main driver for biogeochemical distributions in the open ocean, it reveals the necessity to consider riverine inputs for the representation of heterogeneous features in the coastal ocean and to represent riverine-induced pre-industrial carbon outgassing in the ocean. It also underlines the need to consider long-term CO2 sources from volcanic and shale oxidation fluxes in order to close the framework's atmospheric carbon budget.

Description: The carbon cycle component of the newly developed Earth System Model of intermediate complexity CLIMBER-X is presented. The model represents the cycling of carbon through atmosphere, vegetation, soils, seawater and marine sediments. Exchanges of carbon with geological reservoirs occur through sediment burial, rock weathering and volcanic degassing. The state-of-the-art HAMOCC6 model is employed to simulate ocean biogeochemistry and marine sediments processes. The land model PALADYN simulates the processes related to vegetation and soil carbon dynamics, including permafrost and peatlands. The dust cycle in the model allows for an interactive determination of the input of the micro-nutrient iron into the ocean. A rock weathering scheme is implemented into the model, with the weathering rate depending on lithology, runoff and soil temperature. CLIMBER-X includes a simple representation of the methane cycle, with explicitly modelled natural emissions from land and the assumption of a constant residence time of CH4 in the atmosphere. Carbon isotopes 13C and 14C are tracked through all model compartments and provide a useful diagnostic for model-data comparison. A comprehensive evaluation of the model performance for present–day and the historical period shows that CLIMBER-X is capable of realistically reproducing the historical evolution of atmospheric CO2 and CH4, but also the spatial distribution of carbon on land and the 3D structure of biogeochemical ocean tracers. The analysis of model performance is complemented by an assessment of carbon cycle feedbacks and model sensitivities compared to state-of-the-art CMIP6 models. Enabling interactive carbon cycle in CLIMBER-X results in a relatively minor slow-down of model computational performance by ~20 %, compared to a throughput of ~10,000 simulation years per day on a single node with 16 CPUs on a high performance computer in a climate–only model setup. CLIMBER-X is therefore well suited to investigate the feedbacks between climate and the carbon cycle on temporal scales ranging from decades to 〉100,000 years.

Description: According to modelling studies, ocean alkalinity enhancement (OAE) is one of the proposed carbon dioxide removal (CDR) approaches with large potential, with the beneficial side effect of counteracting ocean acidification. The real-world application of OAE, however, remains unclear as most basic assumptions are untested. Before large-scale deployment can be considered, safe and sustainable procedures for the addition of alkalinity to seawater must be identified and governance established. One of the concerns is the stability of alkalinity when added to seawater. The surface ocean is already supersaturated with respect to calcite and aragonite, and an increase in total alkalinity (TA) together with a corresponding shift in carbonate chemistry towards higher carbonate ion concentrations would result in a further increase in supersaturation, and potentially to solid carbonate precipitation. Precipitation of carbonate minerals consumes alkalinity and increases dissolved CO2 in seawater, thereby reducing the efficiency of OAE for CO2 removal. In order to address the application of alkaline solution as well as fine particulate alkaline solids, a set of six experiments was performed using natural seawater with alkalinity of around 2400 µmol kgsw−1. The application of CO2-equilibrated alkaline solution bears the lowest risk of losing alkalinity due to carbonate phase formation if added total alkalinity (ΔTA) is less than 2400 µmol kgsw−1. The addition of reactive alkaline solids can cause a net loss of alkalinity if added ΔTA 〉 600 µmol kgsw−1 (e.g. for Mg(OH)2). Commercially available (ultrafine) Ca(OH)2 causes, in general, a net loss in TA for the tested amounts of TA addition, which has consequences for suggested use of slurries with alkaline solids supplied from ships. The rapid application of excessive amounts of Ca(OH)2, exceeding a threshold for alkalinity loss, resulted in a massive increase in TA (〉 20 000 µmol kgsw−1) at the cost of lower efficiency and resultant high pH values 〉 9.5. Analysis of precipitates indicates formation of aragonite. However, unstable carbonate phases formed can partially redissolve, indicating that net loss of a fraction of alkalinity may not be permanent, which has important implications for real-world OAE application. Our results indicate that using an alkaline solution instead of reactive alkaline particles can avoid carbonate formation, unless alkalinity addition via solutions shifts the system beyond critical supersaturation levels. To avoid the loss of alkalinity and dissolved inorganic carbon (DIC) from seawater, the application of reactor techniques can be considered. These techniques produce an equilibrated solution from alkaline solids and CO2 prior to application. Differing behaviours of tested materials suggest that standardized engineered materials for OAE need to be developed to achieve safe and sustainable OAE with solids, if reactors technologies should be avoided.

Description: Ocean alkalinity enhancement (OAE) is considered for the long-term removal of gigatons of carbon dioxide (CO2) from the atmosphere to achieve our climate goals. Little is known, however, about the ecosystem-level changes in biogeochemical functioning that may result from the chemical sequestration of CO2 in seawater, and how stable the sequestration is. We studied these two aspects in natural plankton communities under carbonate-based, CO2-equilibrated OAE in the nutrient-poor North Atlantic. During a month-long mesocosm experiment, the majority of biogeochemical pools, including inorganic nutrients, particulate organic carbon and phosphorus as well as biogenic silica, remained unaltered across all OAE levels of up to a doubling of ambient alkalinity (+2400 µeq kg-1). Noticeable exceptions were a minor decrease in particulate organic nitrogen and an increase in the carbon to nitrogen ratio (C:N) of particulate organic matter in response to OAE. Thus, in our nitrogen limited system, nitrogen turnover processes appear more susceptible than those of other elements leading to decreased food quality and increased organic carbon storage. However, alkalinity and chemical CO2 sequestration were not stable at all levels of OAE. Two weeks after alkalinity addition, we measured a loss of added alkalinity and of the initially stored CO2 in the mesocosm where alkalinity was highest (+2400 µeq kg-1, Ωaragonite ~10). The loss rate accelerated over time. Additional tests showed that such secondary precipitation can be initiated by particles acting as precipitation nuclei and that this process can occur even at lower levels of OAE. In conclusion, on the one hand, our study under carbonate-based OAE where the carbon is already sequestered, the risk of major and sustained impacts on biogeochemical functioning may be low in the nutrient-poor ocean. On the other hand, the durability of carbon sequestration using OAE could be constrained by alkalinity loss in supersaturated waters with precipitation nuclei present. Our study provides evaluation of ecosystem impacts of an idealised OAE deployment for monitoring, reporting and verification (MRV) in an oligotrophic system. Whether biogeochemical functioning is resilient to more technically simple and economically more viable approaches that induce stronger water chemistry perturbations remains to be seen.