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Carbon dioxide removal (CDR) technologies at a gigaton scale need to be developed and implemented within the next decades to keep global warming below 1.5 °C. Coastal enhanced silicate weathering is one of the proposed CDR techniques that aims to accelerate the natural process of CO 2 -sequestration during marine chemical weathering of silicate minerals. To this end, finely ground rock containing olivine (Mg x Fe 2− x SiO 4) could be dispersed in dynamic coastal environments, where local biotic and abiotic factors potentially enhance the weathering process. However, accurate predictions of the olivine dissolution rate and the associated CO 2 sequestration under in situ conditions are currently lacking and ecosystem impacts remain to be assessed. Previously, it has been hypothesized that in situ grain collisions, induced by bed load transport due to currents and waves, could accelerate the in situ chemical weathering of olivine particles. To examine this, we investigated the effects of continuous grain tumbling on olivine dissolution in natural seawater. A 70-day experiment was conducted in which forsterite olivine sand was continuously tumbled in filtered seawater at different rotation speeds, and dissolution rates were measured on a weekly basis. Results showed that continuously tumbled olivine dissolved 8 to 19 times faster compared to stagnant (no rotation) conditions. Olivine dissolution was complete and stoichiometric (except for Ni release), air-seawater CO 2 exchange was not significantly rate limiting, and minimal particle fragmentation and secondary mineral formation were observed. Hence, we infer that olivine weathering was mainly enhanced via advective pore water flushing, which limits saturation effects at the grain scale. Overall, this study provides evidence that ambient physical stresses in coastal environments could enhance marine silicate weathering, which has implications for both the natural silicon cycle as well as the use of enhanced coastal weathering of silicates as a CDR technique. [ABSTRACT FROM AUTHOR]

The work assesses the availability and localizations of different raw materials suitable for ocean alkalinity enhancement (OAE), like limestone, olivine, magnesite and brucite, since several billion tons of rocky materials are needed to achieve meaningful results for carbon sequestration through OAE. Resources of carbonates are immense and widespread around all continents. Availability of pure carbonates is still very large (outcrop area 4.1 million km2) and is not a constraint for the large‐scale development of OAE. Outcrops of pure carbonates within 10 km from the coastline and below bare ground or scrub/shrub, preferred for the logistics of exploitation, account for about 70,000 km2, and could provide about 5,000 Gt of limestone. These values increase by a factor of 3 and 8 within 50 and 100 km from the coastline, respectively. Potential resources of olivine, less easily identifiable from the geological data, are estimated in the order of a few hundred billion tons and could provide only a minor contribution to ocean‐based carbon removal strategies. A comparison with the current level of world extraction of mineral raw materials is also provided. The annual production of limestone, estimated to be more than 6.6 Gt from deposits scattered all around the world, is about 9% of the world production of mineral raw materials (around 44 Gt yr−1), and is of the same order of magnitude as coal (7.3 Gt yr−1). The annual productions of magnesite (29 Mt yr−1), olivine (8.4 Mt yr−1) and brucite (1.5 Mt yr−1) are two orders of magnitude lower. Plain Language Summary: The ongoing acidification of the oceans due to the increase of carbon dioxide (CO2) concentration in the atmosphere and the consequent increased uptake by the sea can be tackled by adding alkaline compounds under controlled conditions. Since this promotes a number of reactions in the carbonate system which ultimately results in a drawdown of atmospheric CO2, the enhancement of ocean alkalinity can also contribute to the global effort of limiting global warming, and it is widely studied in the literature among the CO2 removal technologies. A limiting factor can be the worldwide availability of alkaline materials to be used for such a scope. The paper shows that the global availability of pure carbonates is vast, although unevenly distributed, and it could largely satisfy the requirement for large‐scale development of ocean alkalinization. The required up‐scaling of limestone production compared to the current level is much lower than what would be needed for other raw materials that could be used, such as olivine, magnesite and brucite. Moreover, a large fraction of pure limestone resources that could be exploitable is located nearby the coastline, in areas without or with low vegetation cover, which favors the logistics related to the exploitation. Key Points: Pure carbonate potential resources are of several trillion tons and are not a constraint for the development of global‐scale ocean limingA large part of pure limestone resources is located nearby the coastline, in area with no to low vegetation cover, mainly in North Africa and IranThe global limestone yearly production is similar to that of coal, thus the needed upscale is far lower than for olivine, magnesite and brucite [ABSTRACT FROM AUTHOR]

Long-term variations in ocean acidification indices in the Northwest Pacific were examined using observational data and a biogeochemical model with an operational ocean model product for the period 1993–2018. The model and observational data for the surface ocean (< 100-m depth) exhibit consistent patterns of ocean acidification in the subtropical and Kuroshio Extension regions and relative alkalinization (i.e., reduced acidification) in the subarctic region of the Northwest Pacific. Below 100-m depth, acidification dominated in the subtropical regions and alkalinization in the subarctic regions. We attribute the excess acidification in the subtropical and Kuroshio regions to the vertical mixing of dissolved inorganic carbon (DIC) exceeding the DIC release by air–sea exchange. These regional differences in acidification and alkalinization are attributed to spatially variable biological processes in the upper ocean and horizontal and vertical physical redistribution of DIC. Our model and observational results have implications for the spatial extent and pattern of ocean acidification, along with the strength of the ocean carbon sink, which are key aspects of global climate change. [ABSTRACT FROM AUTHOR]

It is now widely recognized that in order to reach the target of limiting global warming to well below 2°C above pre-industrial levels (as the objective of the Paris agreement), cutting the carbon emissions even at an unprecedented pace will not be sufficient, but there is the need for development and implementation of active Carbon Dioxide Removal (CDR) strategies. Among the CDR strategies that currently exist, relatively few studies have assessed the mitigation capacity of ocean-based Negative Emission Technologies (NET) and the feasibility of their implementation on a larger scale to support efficient implementation strategies of CDR. This study investigates the case of ocean alkalinization, which has the additional potential of contrasting the ongoing acidification resulting from increased uptake of atmospheric CO2 by the seas. More specifically, we present an analysis of marine alkalinization applied to the Mediterranean Sea taking into consideration the regional characteristics of the basin. Rather than using idealized spatially homogenous scenarios of alkalinization as done in previous studies, which are practically hard to implement, we use a set of numerical simulations of alkalinization based on current shipping routes to quantitatively assess the alkalinization efficiency via a coupled physical-biogeochemical model (NEMO-BFM) for the Mediterranean Sea at 1/16° horizontal resolution (~6 km) under an RCP4.5 scenario over the next decades. Simulations suggest the potential of nearly doubling the carbon-dioxide uptake rate of the Mediterranean Sea after 30 years of alkalinization, and of neutralizing the mean surface acidification trend of the baseline scenario without alkalinization over the same time span. These levels are achieved via two different alkalinization strategies that are technically feasible using the current network of cargo and tanker ships: a first approach applying annual discharge of 200 Mt Ca(OH)2 constant over the alkalinization period and a second approach with gradually increasing discharge proportional to the surface pH trend of the baseline scenario, reaching similar amounts of annual discharge by the end of the alkalinization period. We demonstrate that the latter approach allows to stabilize the mean surface pH at present day values and substantially increase the potential to counteract acidification relative to the alkalinity added, while the carbon uptake efficiency (mole of CO2 absorbed by the ocean per mole of alkalinity added) is only marginally reduced. Nevertheless, significant local alterations of the surface pH persist, calling for an investigation of the physiological and ecological implications of the extent of these alterations to the carbonate system in the short to medium term in order to support a safe, sustainable application of this CDR implementation.

The effectiveness, feasibility, duration of effects, co-benefits, disbenefits, cost effectiveness and governability of four ocean-based negative emissions technologies (NETs) are assessed in comparison to eight other ocean-based measures. Their role in revising UNFCCC Parties' future Nationally Determined Contributions is discussed in the broad context of ocean-based actions for both mitigation and ecological adaptation. All measures are clustered in three policy-relevant categories (Decisive, Low Regret, Concept Stage). None of the ocean-based NETs assessed are identified as Decisive at this stage. One is Low Regret (Restoring and increasing coastal vegetation), and three are at Concept Stage, one with low to moderate potential disbenefits (Marine bioenergy with carbon capture and storage) and two with potentially high disbenefits (Enhancing open-ocean productivity and Enhancing weathering and alkalinization). Ocean-based NETs are uncertain but potentially highly effective. They have high priority for research and development.

Abstract To monitor the success of carbon dioxide removal (CDR) or solar radiation management (SRM) that offset anthropogenic climate change, the forced response to any external forcing is required to be detectable against internal variability. Thus far, only the detectability of SRM has been examined using both a stationary and nonstationary detection and attribution method. Here, the spatiotemporal detectability of the forced response to artificial ocean alkalinization (AOA) and stratospheric aerosol injection (SAI) as exemplary methods for CDR and SRM, respectively, is compared in Max Planck Institute Earth System Model (MPI‐ESM) experiments using regularized optimal fingerprinting and single‐model estimates of internal variability, while working under a stationary or nonstationary null hypothesis. Although both experiments are forced by emissions according to the Representative Concentration Pathway 8.5 (RCP8.5) and target the climate of the RCP4.5 scenario using AOA or SAI, detection timescales reflect the fundamentally different forcing agents. Moreover, detectability timescales are sensitive to the choice of null hypothesis. Globally, changes in the CO2 system in seawater are detected earlier than the response in temperature to AOA but later in the case of SAI. Locally, the detection time scales depend on the physical, chemical, and radiative impacts of CDR and SRM forcing on the climate system, as well as patterns of internal variability, which is highlighted for oceanic heat and carbon storage.

To monitor the success of carbon dioxide removal (CDR) or solar radiation management (SRM) that offset anthropogenic climate change, the forced response to any external forcing is required to be detectable against internal variability. Thus far, only the detectability of SRM has been examined using both a stationary and nonstationary detection and attribution method. Here, the spatiotemporal detectability of the forced response to artificial ocean alkalinization (AOA) and stratospheric aerosol injection (SAI) as exemplary methods for CDR and SRM, respectively, is compared in Max Planck Institute Earth System Model (MPI‐ESM) experiments using regularized optimal fingerprinting and single‐model estimates of internal variability, while working under a stationary or nonstationary null hypothesis. Although both experiments are forced by emissions according to the Representative Concentration Pathway 8.5 (RCP8.5) and target the climate of the RCP4.5 scenario using AOA or SAI, detection timescales reflect the fundamentally different forcing agents. Moreover, detectability timescales are sensitive to the choice of null hypothesis. Globally, changes in the CO2 system in seawater are detected earlier than the response in temperature to AOA but later in the case of SAI. Locally, the detection time scales depend on the physical, chemical, and radiative impacts of CDR and SRM forcing on the climate system, as well as patterns of internal variability, which is highlighted for oceanic heat and carbon storage. Key Points: Detectability is robust using regularized optimal fingerprinting and single‐model estimates of internal variabilityChanges in the CO2 system in seawater are detected earlier than the thermodynamic response to AOA but later in the case of SAILocal detectability depends on patterns of internal variability and physical, chemical, and radiative impacts of external forcing [ABSTRACT FROM AUTHOR]

A new process to remove carbon dioxide (CO2) from the atmosphere, by combining commercial industrial technologies with ocean liming and CO2 storage, is presented. The process aims to overcome the limiting factors of other negative emission technologies (cost and energy requirements, potential competition for land and freshwater) while simultaneously addressing the problem of ocean acidification. The overall proposed process is based on the following: (a) a gasifier where the biomass is converted to syngas; (b) a thermal steam reformer working at high temperature where the hydrocarbons and tar oils are converted to hydrogen (H2) and carbon monoxide (CO); (c) a kiln to produce Ca(OH)2 (slaked lime) from limestone by using the enthalpy of the hot syngas; (d) the spreading, by means of vessels, of the slaked lime into the seawater to achieve ocean liming; (e) the delivery of syngas to a water gas shift reactor producing CO2 and H2 that are then separated; (f) the final storage of all CO2 produced in the process; (g) the use of H2, being the valuable by-product of the whole process, for decarbonized energy production as well as for ammonia synthesis, offsetting part of the production cost, thus generating "low-cost" negative emissions. The mass and energy balances show that the total atmospheric CO2 removed by the process is 2.6 ton per ton of biomass used. By adding an estimated 0.43 ton avoided—thanks to the use of produced H2—the overall CO2 benefit of the process increases to 3.0 ton per ton of biomass. A preliminary cost analysis resulted in an average levelized cost of 98 $ per ton of CO2 removed; when considering the revenues from the produced energy, the cost falls to 64 $/tCO2. The higher efficiency in carbon removal obtained allows to reduce the amount of biomass required by BECCS (bioenergy with carbon capture and storage) to achieve negative emissions, and thanks to the valuable H2 produced it lowers the costs of CO2 removal from the atmosphere. [ABSTRACT FROM AUTHOR]

Abstract: The potential of coastal ocean alkalinization (COA), a carbon dioxide removal (CDR) climate engineering strategy that chemically increases ocean carbon uptake and storage, is investigated with an Earth system model of intermediate complexity. The CDR potential and possible environmental side effects are estimated for various COA deployment scenarios, assuming olivine as the alkalinity source in ice‐free coastal waters (about 8.6% of the global ocean's surface area), with dissolution rates being a function of grain size, ambient seawater temperature, and pH. Our results indicate that for a large‐enough olivine deployment of small‐enough grain sizes (10 µm), atmospheric CO2 could be reduced by more than 800 GtC by the year 2100. However, COA with coarse olivine grains (1000 µm) has little CO2 sequestration potential on this time scale. Ambitious CDR with fine olivine grains would increase coastal aragonite saturation Ω to levels well beyond those that are currently observed. When imposing upper limits for aragonite saturation levels (Ωlim) in the grid boxes subject to COA (Ωlim = 3.4 and 9 chosen as examples), COA still has the potential to reduce atmospheric CO2 by 265 GtC (Ωlim = 3.4) to 790 GtC (Ωlim = 9) and increase ocean carbon storage by 290 Gt (Ωlim = 3.4) to 913 Gt (Ωlim = 9) by year 2100. [ABSTRACT FROM AUTHOR]

• Olivine exposure results in significant Ni and Cr accumulation in Gammarus locusta. • Metal bioaccumulation was dependent on olivine grain size and concentration. • Chronic reproductive toxicity occurred at 10% w/w olivine. • Ecosystem impacts could limit the scale of coastal enhanced olivine weathering. Active atmospheric carbon dioxide removal (CDR) is needed at a gigaton scale in the next decades to keep global warming below 1.5 °C. Coastal enhanced silicate weathering (CESW) aims to increase natural ocean carbon sequestration via chemical weathering of finely ground olivine (Mg x Fe (1− x) SiO 4) rich rock dispersed in dynamic coastal environments. However, the environmental safety of the technique remains in question due to the high Ni and Cr content of olivine. Therefore, we investigated the short term bioaccumulation and chronic toxicity of olivine in the marine amphipod Gammarus locusta. Acute 24-h olivine exposure resulted in significant grain size dependent olivine ingestion and subsequent Ni and Cr accumulation in tissues. Thousands of small (mainly ≤ 10 µm) olivine grains were ingested by G. locusta , but their importance for trace metal bioaccumulation requires additional research. Most olivine grains were egested within 24 h. Chronic 35-day olivine (3–99 µm) exposure reduced amphipod survival, growth, and reproduction, likely as a result of metal induced oxidative stress and disturbance of major cation homeostasis. Amphipod reproduction was significantly reduced at olivine concentrations of 10% w/w and higher. In the context of ecological risk assessment, application of an arbitrary assessment factor of 100 to the highest no observed effect concentration of 1% w/w olivine yields a very low predicted no-effect concentration (PNEC) of 0.01% w/w olivine. This low PNEC value highlights the urgent need for additional marine olivine toxicity data to accurately assess the environmentally safe scale of coastal enhanced weathering for climate change mitigation. [Display omitted] [ABSTRACT FROM AUTHOR]

Artificial ocean alkalinization (AOA) is investigated as a method to mitigate local ocean acidification and protect tropical coral ecosystems during a 21st century high CO _2 emission scenario. Employing an Earth system model of intermediate complexity, our implementation of AOA in the Great Barrier Reef, Caribbean Sea and South China Sea regions, shows that alkalinization has the potential to counteract expected 21st century local acidification in regard to both oceanic surface aragonite saturation Ω and surface pCO _2 . Beyond preventing local acidification, regional AOA, however, results in locally elevated aragonite oversaturation and pCO _2 decline. A notable consequence of stopping regional AOA is a rapid shift back to the acidified conditions of the target regions. We conclude that AOA may be a method that could help to keep regional coral ecosystems within saturation states and pCO _2 values close to present-day values even in a high-emission scenario and thereby might ‘buy some time’ against the ocean acidification threat, even though regional AOA does not significantly mitigate the warming threat.

Ongoing global warming induced by anthropogenic emissions has opened the debate as to whether geoengineering is a ‘quick fix’ option. Here we analyse the intended and unintended effects of one specific geoengineering approach, which is enhanced weathering via the open ocean dissolution of the silicate-containing mineral olivine. This approach would not only reduce atmospheric CO _2 and oppose surface ocean acidification, but would also impact on marine biology. If dissolved in the surface ocean, olivine sequesters 0.28 g carbon per g of olivine dissolved, similar to land-based enhanced weathering. Silicic acid input, a byproduct of the olivine dissolution, alters marine biology because silicate is in certain areas the limiting nutrient for diatoms. As a consequence, our model predicts a shift in phytoplankton species composition towards diatoms, altering the biological carbon pumps. Enhanced olivine dissolution, both on land and in the ocean, therefore needs to be considered as ocean fertilization. From dissolution kinetics we calculate that only olivine particles with a grain size of the order of 1 μm sink slowly enough to enable a nearly complete dissolution. The energy consumption for grinding to this small size might reduce the carbon sequestration efficiency by ∼30%.

Enhanced silicate weathering (ESW) by spreading finely ground silicate rock along the coastal zone to remove atmospheric carbon dioxide (CO 2 ) is a proposed climate change mitigation technique. The abundant and fast-dissolving mineral olivine has received the most attention for this application. However, olivine contains nickel (Ni) and chromium (Cr), which may pose a risk to marine biota during a gigaton-scale ESW application. Herein we derive a first guideline for coastal olivine dispersal based on existing marine environmental quality standards (EQS) for Ni and Cr. Results show that benthic biota are at the highest risk when olivine and its associated trace metals are mixed in the surface sediment. Specifically, depending on local sedimentary Ni concentrations, 0.059-1.4 kg of olivine m -2 of seabed could be supplied without posing risks for benthic biota. Accordingly, globally coastal ESW could safely sequester only 0.51-37 Gt of CO 2 in the 21st century. On the basis of current EQS, we conclude that adverse environmental impacts from Ni and Cr release could reduce the applicability of olivine in coastal ESW. Our findings call for more in-depth studies on the potential toxicity of olivine toward benthic marine biota, especially in regard to bioavailability and metal mixture toxicity.