Atmospheric methane is a potent greenhouse gas that is photochemically active. The addition of chlorine to the atmosphere has been proposed to mitigate global warming through methane reduction by increasing its chemical loss. However, the potential environmental impacts of such climate mitigation remain unexplored. We explore the possible effects of increasing reactive chlorine emissions on the methane budget, atmospheric composition and radiative forcing. Due to non-linear chemistry we found that achieving effective methane reduction require a minimum 3-fold increase in chlorine atoms compared to present-day levels. Our highest scenario, 50-fold present-day chlorine levels, led to a reduction of the surface temperature by 0.6°C in the year 2050. Beyond the direct effects on methane and temperature, our results show significant alterations in other climate forcers, particularly a large decrease in tropospheric ozone. This translates into a reduction in radiative forcing of a similar magnitude as of the methane removed. Additionally, the Antarctic stratosphere ozone burden during September and October was reduced by up to 40% with the highest chlorine addition. Consequently, the implementation of such strategies requires careful consideration of various factors, including the quantity and method of chlorine addition, as well as potential environmental impacts on air quality and ocean acidity.
Palmer Deep submarine canyon on the western Antarctic Peninsula hosts permanent penguin breeding rookeries and is characterized by elevated chlorophyll-a compared to the surrounding continental shelf. Particle residence times within the canyon are shorter than phytoplankton doubling times, which points to the ecosystem's productivity being tied primarily to advection of externally generated biomass into the canyon. This view is supported by recent observational studies showing alignment of attractive flow structures with phytoplankton patches. While residence times are short, they vary in space and are longer than the timescale for submesoscale instabilities with strong vertical motions (an inertial period), allowing for biological sources to be regionally or episodically important. Here we use measurements of ocean surface velocities (from high-frequency radars) and chlorophyll (from satellites) to calculate the Eulerian, Lagrangian, and horizontal advection terms of the surface chlorophyll budget. The Lagrangian term (including biological sources) is generally comparable in magnitude to advection, but the latter is more important on the canyon's western flank. We then compare joint distributions of relative vorticity and strain conditioned on a particle's net chlorophyll change. In general, parcels experiencing a net increase (decrease) in chlorophyll experience greater cyclonic (anticyclonic) vorticity. Although high-vorticity features significantly influence parcel motion, trajectories generally align with an estimate of the balanced flow, which is often characterized by a cyclone over the central canyon and eastern flank. Without subsurface data we cannot confirm whether the Lagrangian change truly indicates biological accumulation but we offer some interpretations.
The Southern Ocean has long been known to be an important region for ocean CO2 uptake, and one which is especially sensitive to changes in the overlying climate. Here we assess the Southern Ocean CO2 uptake (1985–2018) using data sets gathered in the REgional Carbon Cycle Assessment and Processes Project Phase 2 (RECCAP2). These include global ocean biogeochemical models (GOBMs), surface ocean pCO2-products, data-assimilated models, and interior ocean biogeochemical observations. Over this period the Southern Ocean acted as a sink for CO2, with magnitudes which are roughly half of those reported by RECCAP1 for the same region and timeframe. Close agreement is found between GOBMs and pCO2-products, partly due to some compensation of seasonal and regional differences. Seasonal analyses revealed agreement in driving processes in winter (with uncertainty in the magnitude of outgassing), whereas discrepancies are more fundamental in summer, when GOBMs exhibit difficulties in simulating the balance of non-thermal processes of biology and mixing/circulation. The data sets emphasize strong latitudinal variations in the mean and seasonality of the CO2 flux and asymmetries in the mean and amplitude of the CO2 flux between Atlantic, Pacific and Indian sectors. The present-day net uptake is to first order a response to rising atmospheric CO2. This drives large amounts of anthropogenic CO2 (Cant) into the ocean, thereby overcompensating the loss of natural CO2 to the atmosphere driven by the changing climate. The GOBMs show, however, a 20% spread and an overall underestimate of Cant storage in the ocean interior. An apparent knowledge gap is the increase of the sink since 2000, with pCO2-products suggesting a growth that is more than twice as strong and uncertain as that of GOBMs. This is despite nearly identical pCO2 trends in GOBMs and pCO2-products when both products are compared only at the locations where pCO2 was measured.
Construction materials generate nearly one-third of global carbon emissions, yet conventional accounting captures only a fraction of this impact. Using EXIOBASE data spanning 25 years, we tracked emissions across construction supply chains for cement, steel, metals, and plastics. While global construction demand nearly tripled, regional patterns diverged significantly. The EU reduced emissions despite increased demand through renewable energy adoption and emissions trading, while China's construction boom-driving most global growth-significantly increased domestic emissions. Manufacturing contributes most to embodied emissions compared to resource extraction and waste treatment. Increased reliance on offshore production undermines domestic emission control strategies, highlighting the need for expanded carbon border adjustment mechanisms. Without policies addressing full supply chain emissions, even aggressive climate initiatives will be compromised by carbon leakage, creating an emissions trajectory incompatible with global climate targets.
The distribution of helium isotopes in the upper kilometer of the water column along the GP15 section in the central Pacific reflects the large-scale patterns of upwelling hydrothermal 3He in the tropics and sub-polar gyre, tracing two important pathways whereby bottom water exits from the deep Pacific. Heavy noble gas saturation anomalies, particularly in the upper two hundred meters of the water column, are more strongly increased by seasonal radiative heating, while lighter noble gas saturation anomalies are increased more by air injection processes. A similar, seasonally persistent radiative heating feature was observed in the Equatorial Undercurrent, and appears to be replicated in climate system model simulations. The origin of this feature, however, remains a mystery. A heuristic component model explains the noble gas saturation anomaly distributions, separating the influences of air injection, barometric pressure and radiative heating/cooling. Results show cohesive spatial patterns consistent with where water masses originate, their circulation, and gas exchange dynamics in relation to their formation regions. Using this model, we diagnose the distribution of "non-atmospheric" 4He in shallow waters, which parallels the helium isotope anomaly and silica distributions.
To achieve net zero carbon emissions by mid-century, the United States may need to rely on carbon dioxide removal (CDR) to offset emissions from difficult-to-decarbonize sectors and/or shortfalls in near-term mitigation efforts. CDR can be delivered using many approaches with different requirements for land, water, geologic carbon storage capacity, energy, and other resources. The availability of these resources varies by region in the U.S. suggesting that CDR deployment will be uneven across the country. Using the global change analysis model for the United States (GCAM-USA), we modeled six classes of CDR and explored their potential using four scenarios: a scenario where all the CDR pathways are available (Full Portfolio), a scenario with restricted carbon capture and storage (Low CCS), a scenario where the availability of bio-based CDR options is limited (Low Bio), and a scenario with constraints on enhanced rock weathering (ERW) capabilities (Low ERW). We find that by employing a diverse set of CDR approaches, the U.S. could remove between 1 and 1.9 GtCO _2 /yr by midcentury. In the Full Portfolio scenario, direct air carbon capture and storage (DACCS) predominates, delivering approximately 50% of CO _2 removal, with bioenergy with carbon capture and storage contributing 25%, and ERW delivering 11.5%. Texas and the agricultural Midwest lead in CDR deployment due to their abundant agricultural land and geological storage availability. In the Low CCS scenario, reliance on DACCS decreases, easing pressure on energy systems but increasing pressure on the land. In all cases CDR deployment was found to drive important impacts on energy, land, or materials supply chains (to supply ERW, for example) and these effects were generally more pronounced when fewer CDR technologies were available.
Abstract Recent marine heatwaves in the Gulf of Alaska have had devastating impacts on species from various trophic levels. Due to climate change, total heat exposure in the upper ocean has become longer, more intense, more frequent, and more likely to happen at the same time as other environmental extremes. The combination of multiple environmental extremes can exacerbate the response of sensitive marine organisms. Our hindcast simulation provides the first indication that more than 20% of the bottom water of the Gulf of Alaska continental shelf was exposed to quadruple heat, positive hydrogen ion concentration [H+], negative aragonite saturation state (Ωarag), and negative oxygen concentration [O2] compound extreme events during the 2018–2020 marine heat wave. Natural intrusion of deep and acidified water combined with the marine heat wave triggered the first occurrence of these events in 2019. During the 2013–2016 marine heat wave, surface waters were already exposed to widespread marine heat and positive [H+] compound extreme events due to the temperature effect on the [H+]. We introduce a new Gulf of Alaska Downwelling Index (GOADI) with short‐term predictive skill, which can serve as indicator of past and near‐future positive [H+], negative Ωarag, and negative [O2] compound extreme events near the shelf seafloor. Our results suggest that the marine heat waves may have not been the sole environmental stressor that led to the observed ecosystem impacts and warrant a closer look at existing in situ inorganic carbon and other environmental data in combination with biological observations and model output.
To inform water quality monitoring techniques and modeling at coastal research sites, this study investigated seasonality and trends in coastal lagoons on the eastern shore of Virginia, USA. Seasonality was quantified with harmonic analysis of low-frequency time-series, approximately 30 years of quarterly sampled data at thirteen mainland, lagoon, and ocean inlet sites, along with 4-6 years of high-frequency, 15-min resolution sonde data at two mainland sites. Temperature, dissolved oxygen, and apparent oxygen utilization (AOU) seasonality were dominated by annual harmonics, while salinity and chlorophyll-a exhibited mixed annual and semi-annual harmonics. Mainland sites had larger seasonal amplitudes and higher peak summer values for temperature, chlorophyll-a and AOU, likely from longer water residence times, shallower waters, and proximity to marshes and uplands. Based on the statistical subsampling of high-frequency data, one to several decades of low-frequency data (at quarterly sampling) were needed to quantify the climatological seasonal cycle within specified confidence intervals. Statistically significant decadal warming and increasing chlorophyll-a concentrations were found at a sub-set of mainland sites, with no distinct geographic patterns for other water quality trends. The analysis highlighted challenges in detecting long-term trends in coastal water quality at sites sampled at low frequency with large seasonal and interannual variability.
Interannual variability (IAV) in the atmospheric CO2 growth rate is caused by variation in the balance between uptake by land and ocean and accumulation of anthropogenic emissions in the atmosphere. While variations in terrestrial fluxes are thought to drive most of the observed atmospheric CO2 IAV, the ability to characterize ocean impacts has been limited by the fact that most sites in the surface CO2 monitoring network are located on coasts or islands or within the continental interior. NASA’s Orbiting Carbon-Observatory 2 (OCO-2) mission has observed the atmospheric total column carbon dioxide mole fraction (XCO2) from space since September 2014. With a near-global coverage, this dataset provides a first opportunity to directly observe IAV in atmospheric CO2 over remote ocean regions. We assess the impact of ocean flux IAV on the OCO-2 record using atmospheric transport simulations with underlying gridded air-sea CO2 fluxes from observation-based products. We use three observation-based products to bracket the likely range of ocean air-sea flux contributions to XCO2 variability (over both land and ocean) within the GEOS-Chem atmospheric transport model. We find that the magnitude of XCO2 IAV generated by the whole ocean is between 0.08-0.12 ppm throughout the world. Depending on location and flux product, between 20-80% of the IAV in the simulations is caused by IAV in air-sea CO2 fluxes, with the remainder due to IAV in atmospheric winds, which modulate the atmospheric gradients that arise from climatological ocean fluxes. The Southern Hemisphere mid-latitudes and low-latitudes are the dominant ocean regions in generating the XCO2 IAV globally. The simulation results based on all three flux products show that even within the Northern Hemisphere atmosphere, Southern Hemisphere ocean fluxes are the dominant source of variability in XCO2. Nevertheless, the small magnitude of the air-sea flux impacts on XCO2 presents a substantial challenge for detection of ocean-driven IAV from OCO-2. Although the IAV amplitude arising from ocean fluxes and transport is 20 to 50% of the total observed XCO2 IAV amplitude of 0.4 to 1.6 ppm in the Southern Hemisphere and the tropics, ocean-driven IAV represents only 10% of the observed amplitude in the Northern Hemisphere. We find that for all three products, the simulated ocean-driven XCO2 IAV is weakly anti-correlated with OCO-2 observations, although these correlations are not statistically significant (p>0.05), suggesting that even over ocean basins, terrestrial IAV obscures the ocean signal.
Scenarios to stabilize global climate and meet international climate agreements require rapid reductions in human carbon dioxide (CO2) emissions, often augmented by substantial carbon dioxide removal (CDR) from the atmosphere. While some ocean-based removal techniques show potential promise as part of a broader CDR and decarbonization portfolio, no marine approach is ready yet for deployment at scale because of gaps in both scientific and engineering knowledge. Marine CDR spans a wide range of biotic and abiotic methods, with both common and technique-specific limitations. Further targeted research is needed on CDR efficacy, permanence, and additionality as well as on robust validation methods—measurement, monitoring, reporting, and verification—that are essential to demonstrate the safe removal and long-term storage of CO2. Engineering studies are needed on constraints including scalability, costs, resource inputs, energy demands, and technical readiness. Research on possible co-benefits, ocean acidification effects, environmental and social impacts, and governance is also required.
High-latitude pelagic marine ecosystems are vulnerable to climate change because of the intertwining of sea/continental ice dynamics, physics, biogeochemistry, and food-web structure. Data from the West Antarctic Peninsula allow us to assess how ice influences marine food webs by modulating solar inputs to the ocean, inhibiting wind mixing, altering the freshwater balance and ocean stability, and providing a physical substrate for organisms. State changes are linked to an increase in storm forcing and changing distribution of ocean heat. Changes ripple through the plankton, shifting the magnitude of primary production and its community composition, altering the abundance of krill and other prey essential for marine mammals and seabirds. These climate-driven changes in the food web are being exacerbated by human activity.
Keeping global surface temperatures below international climate targets will require substantial measures to control atmospheric CO _2 and CH _4 concentrations. Recent studies have focused on interventions to decrease CH _4 through enhanced atmospheric oxidation. Here for the first time using a set of models, we evaluate the effect of adding iron aerosols to the atmosphere to enhance molecular chlorine production, and thus enhance the atmospheric oxidation of methane and reduce its concentration. Using different iron emission sensitivity scenarios, we examine the potential role and impact of enhanced iron emissions on direct interactions with solar radiation, and on the chemical and radiative response of methane. Our results show that the impact of iron emissions on CH _4 depends sensitively on the location of the iron emissions. In all emission regions there is a threshold in the amount of iron that must be added to remove methane. Below this threshold CH _4 increases. Even once that threshold is reached, the iron-aerosol driven chlorine-enhanced impacts on climate are complex. The radiative forcing of both methane and ozone are decreased in the most efficient regions but the direct effect due to the addition of absorbing iron aerosols tends to warm the planet. Adding any anthropogenic aerosol may also cool the planet due to aerosol cloud interactions, although these are very uncertain, and here we focus on the unique properties of adding iron aerosols. If the added emissions have a similar distribution as current shipping emissions, our study shows that the amount of iron aerosols that must be added before methane decreases is 2.5 times the current shipping emissions of iron aerosols, or 6 Tg Fe yr ^−1 in the most ideal case examined here. Our study suggests that the photoactive fraction of iron aerosols is a key variable controlling the impact of iron additions and poorly understood. More studies of the sensitivity of when, where and how iron aerosols are added should be conducted. Before seriously considering this method, additional impacts on the atmospheric chemistry, climate, environmental impacts and air pollution should be carefully assessed in future studies since they are likely to be important.
This study characterized ocean biological carbon pump metrics in the second iteration of the REgional Carbon Cycle Assessment and Processes (RECCAP2) project. The analysis here focused on comparisons of global and biome‐scale regional patterns in particulate organic carbon (POC) production and sinking flux from the RECCAP2 ocean biogeochemical model ensemble against observational products derived from satellite remote sensing, sediment traps, and geochemical methods. There was generally good model‐data agreement in mean large‐scale spatial patterns, but with substantial spread across the model ensemble and observational products. The global‐integrated, model ensemble‐mean export production, taken as the sinking POC flux at 100 m (6.08 ± 1.17 Pg C yr−1), and export ratio defined as sinking flux divided by net primary production (0.154 ± 0.026) both fell at the lower end of observational estimates. Comparison with observational constraints also suggested that the model ensemble may have underestimated regional biological CO2 drawdown and air‐sea CO2 flux in high productivity regions. Reasonable model‐data agreement was found for global‐integrated, ensemble‐mean sinking POC flux into the deep ocean at 1,000 m (0.65 ± 0.24 Pg C yr−1) and the transfer efficiency defined as flux at 1,000 m divided by flux at 100 m (0.122 ± 0.041), with both variables exhibiting considerable regional variability. The RECCAP2 analysis presents standard ocean biological carbon pump metrics for assessing biogeochemical model skill, metrics that are crucial for further modeling efforts to resolve remaining uncertainties involving system‐level interactions between ocean physics and biogeochemistry.
The coastal ocean contributes to regulating atmospheric greenhouse gas concentrations by taking up carbon dioxide (CO2) and releasing nitrous oxide (N2O) and methane (CH4). Major advances have improved our understanding of the coastal air-sea exchanges of these three gasses since the first phase of the Regional Carbon Cycle Assessment and Processes (RECCAP in 2013), but a comprehensive view that integrates the three gasses at the global scale is still lacking. In this second phase (RECCAP2), we quantify global coastal ocean fluxes of CO2, N2O and CH4 using an ensemble of global gap-filled observation-based products and ocean biogeochemical models. The global coastal ocean is a net sink of CO2 in both observational products and models, but the magnitude of the median net global coastal uptake is ~60% larger in models (-0.72 vs. -0.44 PgC/yr, 1998-2018, coastal ocean area of 77 million km2). We attribute most of this model-product difference to the seasonality in sea surface CO2 partial pressure at mid- and high-latitudes, where models simulate stronger winter CO2 uptake. The global coastal ocean is a major source of N2O (+0.70 PgCO2-e /yr in observational product and +0.54 PgCO2-e /yr in model median) and of CH4 (+0.21 PgCO2-e /yr in observational product), which offsets a substantial proportion of the net radiative effect of coastal \co uptake (35-58% in CO2-equivalents). Data products and models need improvement to better resolve the spatio-temporal variability and long term trends in CO2, N2O and CH4 in the global coastal ocean.
The noble gas signature of incoming Pacific Bottom Water (PBW), when compared to North Atlantic Deep Water, indicates the addition of 450 ± 70 GT a −1 glacial melt water to form AABW and subsequently PBW. The downstream evolution of this signature between the southern (20°S to equator) and northern (25°–45°N) bottom waters indicates a decrease in sea level pressure around Antarctica over the past two millennia. Vertical profiles of noble gases in the deep Pacific show exponential relationships with depth with scale heights identical to temperature and salinity. Unlike the other noble gases, helium isotopes show evidence of mid‐depth injection of non‐atmospheric helium. Using observed deviations from exponential behavior, we quantify its magnitude and isotope ratio. There is a clear latitude trend in the isotope ratio of this added helium that decreases from a high exceeding 9 R A (atmospheric 3 He/ 4 He ratio) in the south to around 8 R A near the equator. North of 30–40°N, it systematically decreases northward to a low of ∼2 R A north of 50°N. This decline results from a combination of northward decline in seafloor spreading, release of radiogenic helium from increased sediment thickness, and the possible emission of radiogenic helium through cold seeps along the Alaskan and North American margins. Finally, we derive an improved method of computing the excess helium isotope concentrations and that the distributions of bottom water 3 He XS / 4 He XS are consistent with what is known about bottom water flow patterns and the input of low 3 He/ 4 He sedimentary helium.
The chemical industry is a major and growing source of CO2 emissions. Here, we extend the principal U.S.-based integrated assessment model, GCAM, to include a representation of steam cracking, the dominant process in the organic chemical industry today, and a suite of emerging decarbonization strategies, including catalytic cracking, lower-carbon process heat, and feedstock switching. We find that emerging catalytic production technologies only have a small impact on midcentury emissions mitigation. In contrast, process heat generation could achieve strong mitigation, reducing associated CO2 emissions by ∼76% by 2050. Process heat generation is diversified to include carbon capture and storage (CCS), hydrogen, and electrification. A sensitivity analysis reveals that our results for future net CO2 emissions are most sensitive to the amount of CCS deployed globally. The system as defined cannot reach net-zero emissions if the share of incineration increases as projected without coupling incineration with CCS. Less organic chemicals are produced in a net-zero CO2 future than those in a no-policy scenario. Mitigation of feedstock emissions relies heavily on biogenic carbon used as an alternative feedstock and waste treatment of plastics. The only scenario that delivers net-negative CO2 emissions from the organic chemical sector (by 2070) combines greater use of biogenic feedstocks with a continued reliance on landfilling of waste plastic, versus recycling or incineration, which has trade-offs.
Coastal landscapes are naturally shifting mosaics of distinct ecosystems that are rapidly migrating with sea-level rise. Previous work illustrates that transitions among individual ecosystems have disproportionate impacts on the global carbon cycle, but this cannot address nonlinear interactions between multiple ecosystems that potentially cascade across the coastal landscape. Here, we synthesize carbon stocks, accumulation rates, and regional land cover data over 36 years (1984 and 2020) for a variety of ecosystems across a large portion of the rapidly transgressing mid-Atlantic coast. The coastal landscape of the Virginia Eastern Shore consists of temperate forest, salt marsh, seagrass beds, barrier islands, and coastal lagoons. We found that rapid losses and gains within individual ecosystems largely offset each other, which resulted in relatively stable areas for the different ecosystems, and a 4