Wastewater Treatment for Carbon Dioxide Removal.

Wastewater treatment is notorious for its hefty carbon footprint, accounting for 1-2% of global greenhouse gas (GHG) emissions. Nonetheless, the treatment process itself could also present an innovative carbon dioxide removal (CDR) approach. Here, the calcium (Ca)-rich effluent of a phosphorus (P) recovery system from municipal wastewater (P recovered as calcium phosphate) was used for CDR. The effluent was bubbled with concentrated CO2, leading to its mineralization, i.e., CO2 stored as stable carbonate minerals. The chemical and microstructural properties of the newly formed minerals were ascertained by using state-of-the-art analytical techniques. FTIR identified CO3 bonds and carbonate stretching, XRF and SEM-EDX measured a high Ca concentration, and SEM imaging showed that Ca is well distributed, suggesting homogeneous formation. Furthermore, FIB-SEM revealed rhombohedral and needle-like structures and TEM revealed rod-like structures, indicating that calcium carbonate (CaCO3) was formed, while XRD suggested that this material mainly comprises aragonite and calcite. Results imply that high-quality CaCO3 was synthesized, which could be stored or valorized, while if atmospheric air is used for bubbling, a partial direct air capture (DAC) system could be achieved. The quality of the bubbled effluent was also improved, thus creating water reclamation and circular economy opportunities. Results are indicative of other alkaline Ca-rich wastewaters such as effluents or leachates from legacy iron and steel wastes (steel slags) that can possibly be used for CDR. Overall, it was identified that wastewater can be used for carbon mineralization and can greatly reduce the carbon footprint of the treatment process, thus establishing sustainable paradigms for the introduction of CDR in this sector.

Quantifying CO2 Removal at Enhanced Weathering Sites: a Multiproxy Approach.

Enhanced weathering is a carbon dioxide (CO2) mitigation strategy that promises large scale atmospheric CO2 removal. The main challenge associated with enhanced weathering is monitoring, reporting, and verifying (MRV) the amount of carbon removed as a result of enhanced weathering reactions. Here, we study a CO2 mineralization site in Consett, Co. Durham, UK, where steel slags have been weathered in a landscaped deposit for over 40 years. We provide new radiocarbon, δ13C, 87Sr/86Sr, and major element data in waters, calcite precipitates, and soils to quantify the rate of carbon removal. We demonstrate that measuring the radiocarbon activity of CaCO3 deposited in waters draining the slag deposit provides a robust constraint on the carbon source being sequestered (80% from the atmosphere, 2σ = 8%) and use downstream alkalinity measurements to determine the proportion of carbon exported to the ocean. The main phases dissolving in the slag are hydroxide minerals (e.g., portlandite) with minor contributions (<3%) from silicate minerals. We propose a novel method for quantifying carbon removal rates at enhanced weathering sites, which is a function of the radiocarbon-apportioned sources of carbon being sequestered, and the proportion of carbon being exported from the catchment to the oceans.

Broaden Research on Ocean Alkalinity Enhancement to Better Characterize Social Impacts.

Ocean alkalinity enhancement (OAE) is being considered as a way of achieving large-scale removals of carbon dioxide from the atmosphere. Research on the risks and benefits of different OAE approaches is expanding apace, but it remains difficult to anticipate and appraise the potential impacts to human communities that OAE might generate. These impacts, however, will be critical to evaluating the viability of specific OAE projects. This paper draws on the authors' involvement in interdisciplinary assessment of OAE (1) to identify the factors that currently limit characterization of potential social impacts and (2) to propose ways of reconfiguring OAE research to better consider these.

Life Cycle Assessment of Coastal Enhanced Weathering for Carbon Dioxide Removal from Air.

Coastal enhanced weathering (CEW) is a carbon dioxide removal (CDR) approach whereby crushed silicate minerals are spread in coastal zones to be naturally weathered by waves and tidal currents, releasing alkalinity and removing atmospheric carbon dioxide (CO2). Olivine has been proposed as a candidate mineral due to its abundance and high CO2 uptake potential. A life cycle assessment (LCA) of silt-sized (10 µm) olivine revealed that CEW's life-cycle carbon emissions and total environmental footprint, i.e., carbon and environmental penalty, amount to around 51 kg CO2eq and 3.2 Ecopoint (Pt) units per tonne of captured atmospheric CO2, respectively, and these will be recaptured within a few months. Smaller particle sizes dissolve and uptake atmospheric CO2 even faster; however, their high carbon and environmental footprints (e.g., 223 kg CO2eq and 10.6 Pt tCO2-1, respectively, for 1 µm olivine), engineering challenges in comminution and transportation, and possible environmental stresses (e.g., airborne and/or silt pollution) might restrict their applicability. Alternatively, larger particle sizes exhibit lower footprints (e.g., 14.2 kg CO2eq tCO2-1 and 1.6 Pt tCO2-1, respectively, for 1000 µm olivine) and could be incorporated in coastal zone management schemes, thus possibly crediting CEW with avoided emissions. However, they dissolve much slower, requiring 5 and 37 years before the 1000 µm olivine becomes carbon and environmental net negative, respectively. The differences between the carbon and environmental penalties highlight the need for using multi-issue life cycle impact assessment methods rather than focusing on carbon balances alone. When CEW's full environmental profile was considered, it was identified that fossil fuel-dependent electricity for olivine comminution is the main environmental hotspot, followed by nickel releases, which may have a large impact on marine ecotoxicity. Results were also sensitive to transportation means and distance. Renewable energy and low-nickel olivine can minimize CEW's carbon and environmental profile.

Soil-derived Nature's Contributions to People and their contribution to the UN Sustainable Development Goals.

This special issue provides an assessment of the contribution of soils to Nature's Contributions to People (NCP). Here, we combine this assessment and previously published relationships between NCP and delivery on the UN Sustainable Development Goals (SDGs) to infer contributions of soils to the SDGs. We show that in addition to contributing positively to the delivery of all NCP, soils also have a role in underpinning all SDGs. While highlighting the great potential of soils to contribute to sustainable development, it is recognized that poorly managed, degraded or polluted soils may contribute negatively to both NCP and SDGs. The positive contribution, however, cannot be taken for granted, and soils must be managed carefully to keep them healthy and capable of playing this vital role. A priority for soil management must include: (i) for healthy soils in natural ecosystems, protect them from conversion and degradation; (ii) for managed soils, manage in a way to protect and enhance soil biodiversity, health and sustainability and to prevent degradation; and (iii) for degraded soils, restore to full soil health. We have enough knowledge now to move forward with the implementation of best management practices to maintain and improve soil health. This analysis shows that this is not just desirable, it is essential if we are to meet the SDG targets by 2030 and achieve sustainable development more broadly in the decades to come. This article is part of the theme issue 'The role of soils in delivering Nature's Contributions to People'.

Potential for large-scale CO2 removal via enhanced rock weathering with croplands.

Enhanced silicate rock weathering (ERW), deployable with croplands, has potential use for atmospheric carbon dioxide (CO2) removal (CDR), which is now necessary to mitigate anthropogenic climate change1. ERW also has possible co-benefits for improved food and soil security, and reduced ocean acidification2-4. Here we use an integrated performance modelling approach to make an initial techno-economic assessment for 2050, quantifying how CDR potential and costs vary among nations in relation to business-as-usual energy policies and policies consistent with limiting future warming to 2 degrees Celsius5. China, India, the USA and Brazil have great potential to help achieve average global CDR goals of 0.5 to 2 gigatonnes of carbon dioxide (CO2) per year with extraction costs of approximately US$80-180 per tonne of CO2. These goals and costs are robust, regardless of future energy policies. Deployment within existing croplands offers opportunities to align agriculture and climate policy. However, success will depend upon overcoming political and social inertia to develop regulatory and incentive frameworks. We discuss the challenges and opportunities of ERW deployment, including the potential for excess industrial silicate materials (basalt mine overburden, concrete, and iron and steel slag) to obviate the need for new mining, as well as uncertainties in soil weathering rates and land-ocean transfer of weathered products.

Ambient weathering of magnesium oxide for CO2 removal from air.

To avoid dangerous climate change, new technologies must remove billions of tonnes of CO2 from the atmosphere every year by mid-century. Here we detail a land-based enhanced weathering cycle utilizing magnesite (MgCO3) feedstock to repeatedly capture CO2 from the atmosphere. In this process, MgCO3 is calcined, producing caustic magnesia (MgO) and high-purity CO2. This MgO is spread over land to carbonate for a year by reacting with atmospheric CO2. The carbonate minerals are then recollected and re-calcined. The reproduced MgO is spread over land to carbonate again. We show this process could cost approximately $46-159 tCO2-1 net removed from the atmosphere, considering grid and solar electricity without post-processing costs. This technology may achieve lower costs than projections for more extensively engineered Direct Air Capture methods. It has the scalable potential to remove at least 2-3 GtCO2 year-1, and may make a meaningful contribution to mitigating climate change.

Atmospheric Carbon Capture Performance of Legacy Iron and Steel Waste.

Legacy iron (Fe) and steel wastes have been identified as a significant source of silicate minerals, which can undergo carbonation reactions and thus sequester carbon dioxide (CO2). In reactor experiments, i.e., at elevated temperatures, pressures, or CO2 concentrations, these wastes have high silicate to carbonate conversion rates. However, what is less understood is whether a more "passive" approach to carbonation can work, i.e., whether a traditional slag emplacement method (heaped and then buried) promotes or hinders CO2 sequestration. In this paper, the results of characterization of material retrieved from a first of its kind drilling program on a historical blast furnace slag heap at Consett, U.K., are reported. The mineralogy of the slag material was near uniform, consisting mainly of melilite group minerals with only minor amounts of carbonate minerals detected. Further analysis established that total carbon levels were on average only 0.4% while average calcium (Ca) levels exceeded 30%. It was calculated that only ∼3% of the CO2 sequestration potential of the >30 Mt slag heap has been utilized. It is suggested that limited water and gas interaction and the mineralogy and particle size of the slag are the main factors that have hindered carbonation reactions in the slag heap.

The negative emission potential of alkaline materials.

7 billion tonnes of alkaline materials are produced globally each year as a product or by-product of industrial activity. The aqueous dissolution of these materials creates high pH solutions that dissolves CO2 to store carbon in the form of solid carbonate minerals or dissolved bicarbonate ions. Here we show that these materials have a carbon dioxide storage potential of 2.9-8.5 billion tonnes per year by 2100, and may contribute a substantial proportion of the negative emissions required to limit global temperature change to <2 °C.

Atmospheric CO2 Sequestration in Iron and Steel Slag: Consett, County Durham, United Kingdom.

Carbonate formation in waste from the steel industry could constitute a nontrivial proportion of the global requirements for removing carbon dioxide from the atmosphere at a potentially low cost. To utilize this potential, we examined atmospheric carbon dioxide sequestration in a >20 million ton legacy slag deposit in northern England, United Kingdom. Carbonates formed from the drainage water of the heap had stable carbon and oxygen isotope values between -12 and -25 ‰ and -5 and -18 ‰ for δ13C and δ18O, respectively, suggesting atmospheric carbon dioxide sequestration in high-pH solutions. From the analyses of solution saturation states, we estimate that between 280 and 2900 tons of CO2 have precipitated from the drainage waters. However, by combining a 37 year long data set of the drainage water chemistry with geospatial analysis, we estimate that <1% of the maximum carbon-capture potential of the deposit may have been realized. This implies that uncontrolled deposition of slag is insufficient to maximize carbon sequestration, and there may be considerable quantities of unreacted legacy deposits available for atmospheric carbon sequestration.

Olivine Dissolution in Seawater: Implications for CO2 Sequestration through Enhanced Weathering in Coastal Environments.

Enhanced weathering of (ultra)basic silicate rocks such as olivine-rich dunite has been proposed as a large-scale climate engineering approach. When implemented in coastal environments, olivine weathering is expected to increase seawater alkalinity, thus resulting in additional CO2 uptake from the atmosphere. However, the mechanisms of marine olivine weathering and its effect on seawater-carbonate chemistry remain poorly understood. Here, we present results from batch reaction experiments, in which forsteritic olivine was subjected to rotational agitation in different seawater media for periods of days to months. Olivine dissolution caused a significant increase in alkalinity of the seawater with a consequent DIC increase due to CO2 invasion, thus confirming viability of the basic concept of enhanced silicate weathering. However, our experiments also identified several important challenges with respect to the detailed quantification of the CO2 sequestration efficiency under field conditions, which include nonstoichiometric dissolution, potential pore water saturation in the seabed, and the potential occurrence of secondary reactions. Before enhanced weathering of olivine in coastal environments can be considered an option for realizing negative CO2 emissions for climate mitigation purposes, these aspects need further experimental assessment.

Rapid Removal of Atmospheric CO2 by Urban Soils.

The measured calcium carbonate content of soils to a depth of 100 mm at a large urban development site has increased over 18 months at a rate that corresponds to the sequestration of 85 t of CO2/ha (8.5 kg of CO2 m(-2)) annually. This is a consequence of rapid weathering of calcium silicate and hydroxide minerals derived from the demolition of concrete structures, which releases Ca that combines with CO2 ultimately derived from the atmosphere, precipitating as calcite. Stable isotope data confirm an atmospheric origin for carbonate carbon, and 14C dating indicates the predominance of modern carbon in the pedogenic calcite. Trial pits show that carbonation extends to depths of ≥1 m. Work at other sites shows that the occurrence of pedogenic carbonates is widespread in artificially created urban soils containing Ca and Mg silicate minerals. Appropriate management of fewer than 12000 ha of urban land to maximize calcite precipitation has the potential to remove 1 million t of CO2 from the atmosphere annually. The maximal global potential is estimated to be approximately 700-1200 Mt of CO2 per year (representing 2.0-3.7% of total emissions from fossil fuel combustion) based on current rates of production of industry-derived Ca- and Mg-bearing materials.

Carbon dioxide efficiency of terrestrial enhanced weathering.

Terrestrial enhanced weathering, the spreading of ultramafic silicate rock flour to enhance natural weathering rates, has been suggested as part of a strategy to reduce global atmospheric CO2 levels. We budget potential CO2 sequestration against associated CO2 emissions to assess the net CO2 removal of terrestrial enhanced weathering. We combine global spatial data sets of potential source rocks, transport networks, and application areas with associated CO2 emissions in optimistic and pessimistic scenarios. The results show that the choice of source rocks and material comminution technique dominate the CO2 efficiency of enhanced weathering. CO2 emissions from transport amount to on average 0.5-3% of potentially sequestered CO2. The emissions of material mining and application are negligible. After accounting for all emissions, 0.5-1.0 t CO2 can be sequestered on average per tonne of rock, translating into a unit cost from 1.6 to 9.9 GJ per tonne CO2 sequestered by enhanced weathering. However, to control or reduce atmospheric CO2 concentrations substantially with enhanced weathering would require very large amounts of rock. Before enhanced weathering could be applied on large scales, more research is needed to assess weathering rates, potential side effects, social acceptability, and mechanisms of governance.

Passive sequestration of atmospheric CO2 through coupled plant-mineral reactions in urban soils.

Photosynthetic removal of CO(2) from the atmosphere is an important planetary carbon dioxide removal mechanism. Naturally, an amount equivalent to all atmospheric carbon passes through the coupled plant-soil system within 7 years. Plants cycle up to 40% of photosynthesized carbon through their roots, providing a flux of C at depth into the soil system. Root-exuded carboxylic acids have the potential to supply 4-5 micromoles C hr(-1)g(-1) fresh weight to the soil solution, and enhance silicate mineral weathering. Ultimately, the final product of these root-driven processes is CO(2), present in solution as bicarbonate. This combines with Ca liberated by corrosion associated with silicate mineral weathering to enter the soil-water system and to produce pedogenic calcium carbonate precipitates. Combining understanding of photosynthesis and plant root physiology with knowledge of mineral weathering provides an opportunity to design artificial soils or to plan land use in ways that maximize removal and sequestration of atmospheric CO(2) through artificially enhanced pedogenic carbonate precipitation. This process requires relatively low energy and infrastructure inputs. It offers a sustainable carbon dioxide removal mechanism analogous to the use of constructed wetlands for the passive remediation of contaminated waters, and is likely to achieve wide public acceptance.