Atmospheric CO2 Concentration Research Articles

Investigation on desulfurization and ground granulated blast furnace slags reutilization for carbon dioxide sorption in a fluidized bed reactor

BackgroundThe atmospheric CO2 concentration is significantly increasing due to the utilization of fossil fuel in various activities. Implementation of steel slag is considered as a promising strategy for carbon capture MethodsIn this study, the slags from desulfurization (De-S) and ground granulated blast furnace (GGBS) processes in the steel company waste were applied as the sorbent in CO2 removal using a fluidized bed system. Various operating conditions were applied to determine the influence of operating parameters on sorbent performance. Moreover, examination on sorbent characteristic change and kinetics calculation were also carried out in this study. Significant findingOptimum operating temperature was reached by the application of 600 and 500 °C for De-S and GGBS slag, respectively. The higher CO2 concentration and 5 % water vapor improved the sorbent utilization. However, excessive water vapor and low fluidized velocity decreased the performance of sorbent. De-S slag performed better on overall CO2 capture process compared to GGBS slag. Therefore, upscaled study with 10 times greater size was further conducted with the 150–300 µm De-S slag for the CO2 capture from oxy-fuel and air combustion. The higher CO2 partial pressure in the flue gas of oxy-fuel combustion increased the capture process efficiency.

Has nitrogen availability decreased over much of the land surface in the past century? A model-based analysis

A recent publication (Mason et al. in Science 376:261, 2022a) suggested that nitrogen (N) availability has declined as a consequence of multiple ongoing components of anthropogenic global change. This suggestion is controversial, because human alteration of the global N cycle is substantial and has driven much-increased fixation of N globally. We used a simple model that has been validated across a climate gradient in Hawai ‘i to test the possibility of a widespread decline in N availability, the evidence supporting it, and the possible mechanisms underlying it. This analysis showed that a decrease in δ15N is not sufficient evidence for a decline in N availability, because δ15N in ecosystems reflects both the isotope ratios in inputs of N to the ecosystem AND fractionation of N isotopes as N cycles, with enrichment of the residual N in the ecosystem caused by greater losses of N by the fractionating pathways that are more important in N-rich sites. However, there is other evidence for declining N availability that is independent of 15N and that suggests a widespread decline in N availability. We evaluated whether and how components of anthropogenic global change could cause declining N availability. Earlier work had demonstrated that both increases in the variability of precipitation due to climate change and ecosystem-level disturbance could drive uncontrollable losses of N that reduce N availability and could cause persistent N limitation at equilibrium. Here we modelled climate-change-driven increases in temperature and increasing atmospheric concentrations of CO2. We show that increasing atmospheric CO2 concentrations can drive non-equilibrium decreases in N availability and cause the development of N limitation, while the effects of increased temperature appear to be relatively small and short-lived. These environmental changes may cause reductions in N availability over the vast areas of Earth that are not affected by high rates of atmospheric deposition and/or N enrichment associated with urban and agricultural land use.

Highly stratified mid-Pliocene Southern Ocean in PlioMIP2

Abstract. During the mid-Pliocene warm period (mPWP; 3.264–3.025 Ma), atmospheric CO2 concentrations were approximately 400 ppm, and the Antarctic Ice Sheet was substantially reduced compared to today. Antarctica is surrounded by the Southern Ocean, which plays a crucial role in the global oceanic circulation and climate regulation. Using results from the Pliocene Model Intercomparison Project (PlioMIP2), we investigate Southern Ocean conditions during the mPWP with respect to the pre-industrial period. We find that the mean sea surface temperature (SST) warming in the Southern Ocean is 2.8 °C, while global mean SST warming is 2.4 °C. The enhanced warming is strongly tied to a dramatic decrease in sea ice cover over the mPWP Southern Ocean. We also see a freshening of the ocean (sub)surface, driven by an increase in precipitation over the Southern Ocean and Antarctica. The warmer and fresher surface leads to a highly stratified Southern Ocean that can be related to weakening of the deep abyssal overturning circulation. Sensitivity simulations show that the decrease in sea ice cover and enhanced warming is largely a consequence of the reduction in the Antarctic Ice Sheet. In addition, the mPWP geographic boundary conditions are responsible for approximately half of the increase in mPWP SST warming, sea ice loss, precipitation, and stratification increase over the Southern Ocean. From these results, we conclude that a strongly reduced Antarctic Ice Sheet during the mPWP has a substantial influence on the state of the Southern Ocean and exacerbates the changes that are induced by a higher CO2 concentration alone. This is relevant for the long-term future of the Southern Ocean, as we expect melting of the western Antarctic Ice Sheet in the future, an effect that is not currently taken into account in future projections by Coupled Model Intercomparison Project (CMIP) ensembles.

Carbon dioxide sequestration in cementitious materials: A review of techniques, material performance, and environmental impact

The release of carbon dioxide (CO2) into the earth's atmosphere is a substantial global environmental concern that arises from the processes of industrialization and urbanization. The increase in atmospheric CO2 concentrations has resulted in the phenomenon of global warming and subsequent alterations in climate patterns. Accelerated CO2 sequestration in cementitious materials is currently the subject of extensive research as a highly efficacious approach to mitigating the carbon footprint of the concrete industry. The sequestration procedure entails the transformation of gaseous CO2 into carbonate minerals. The review presented in this paper outlines the most recent carbonation (i.e., CO2 sequestration) techniques, such as mineral carbonation, accelerated CO2 curing (ACC), pre-carbonation, and carbonation mixing, that have been recently explored. The potential of mineral carbonation of industrial wastes and the advantages of their incorporation in the concrete matrix is investigated. Carbonation technologies and their effect on the performance of cementitious composites are reported. Information on life cycle assessment are also included to evaluate the environmental impact associated with the production of carbonated materials. Various commercialized CO2 utilization technologies in construction sector, such as CarbonCure, Solidia, Carbstone, Calera, and Carbon8 are reviewed. Moreover, this review offers a thorough insight into the carbonation technologies, evaluating their advantages, limitations, and the existing gaps in research.

Individual and combined impacts of carbon dioxide enrichment, heatwaves, flow velocity variability, and fine sediment deposition on stream invertebrate communities.

Climate change and land-use change are widely altering freshwater ecosystem functioning and there is an urgent need to understand how these broad stressor categories may interact in future. While much research has focused on mean temperature increases, climate change also involves increasing variability of both water temperature and flow regimes and increasing concentrations of atmospheric CO2, all with potential to alter stream invertebrate communities. Deposited fine sediment is a pervasive land-use stressor with widespread impacts on stream invertebrates. Sedimentation may be managed at the catchment scale; thus, uncovering interactions with these three key climate stressors may assist mitigation of future threats. This is the first experiment to investigate the individual and combined effects of enriched CO2, heatwaves, flow velocity variability, and fine sediment on realistic stream invertebrate communities. Using 128 mesocosms simulating small stony-bottomed streams in a 7-week experiment, we manipulated dissolved CO2 (ambient; enriched), fine sediment (no sediment; 300 g dry sediment), temperature (ambient; two 7-day heatwaves), and flow velocity (constant; variable). All treatments changed community composition. CO2 enrichment reduced abundances of Orthocladiinae and Chironominae and increased Copepoda abundance. Variable flow velocity had only positive effects on invertebrate abundances (7 of 13 common taxa and total abundance), in contrast to previous experiments showing negative impacts of reduced velocity. CO2 was implicated in most stressor interactions found, with CO2 × sediment interactions being most common. Communities forming under enriched CO2 conditions in sediment-impacted mesocosms had ~20% fewer total invertebrates than those with either treatment alone. Copepoda abundances doubled in CO2-enriched mesocosms without sediment, whereas no CO2 effect occurred in mesocosms with sediment. Our findings provide new insights into potential future impacts of climate change and land use in running freshwaters, in particular highlighting the potential for elevated CO2 to interact with fine sediment deposition in unpredictable ways.

Characteristics and drivers of vegetation productivity sensitivity to increasing CO2 at Northern Middle and High Latitudes.

Understanding and accurately predicting how the sensitivity of terrestrial vegetation productivity to rising atmospheric CO2 concentration (β) is crucial for assessing carbon sink dynamics. However, the temporal characteristics and driving mechanisms of β remain uncertain. Here, observational and CMIP6 modeling evidence suggest a decreasing trend in β at the Northern Middle and High Latitudes during the historical period of 1982-2015 (-0.082 ± 0.005% 100 ppm-1 year-1). This decreasing trend is projected to persist until the end of the 21st century (-0.082 ± 0.005% 100 ppm-1 year-1 under SSP370 and -0.166 ± 0.006% 100 ppm-1 year-1 under SSP585). The declining β indicates a weakening capacity of vegetation to mitigate warming climates, posing challenges for achieving the temperature goals of the Paris Agreement. The rise in vapor pressure deficit (VPD), that triggers stomata closure and weakens photosynthesis, is considered as the dominated factor contributing to the historical and future decline in β, accounting for 62.3%-75.2% of the effect. Nutrient availability and water availability contribute 15.7%-21.4% and 8.5%-16.3%, respectively. These findings underscore the significant role of VPD in shaping terrestrial carbon sink dynamics, an aspect that is currently insufficiently considered in many climate and ecological models.

CO2 enrichment accelerates alpine plant growth via increasing water-use efficiency

Phenological changes in global vegetation are often attributed to climate warming. However, climate warming and elevated atmospheric CO2 concentration (eCO2) are two co-occurring global change factors, and how eCO2 would affect vegetation phenology has received less attention. The partial pressure of atmospheric CO2 on the Tibetan Plateau (TP) is lower than that in regions of lower altitudes. Consequently, the growth and phenology of alpine plants in this region could be more sensitive to eCO2, but this hypothesis is not yet supported by empirical evidence. Here we explored the effect of eCO2 on plant phenology (including phenophases of green-up, budding, and flowering) through a 5-year field manipulation experiment in a high-altitude (4600 m above sea level) alpine grassland on the TP. Our results showed that eCO2 significantly advanced the spring phenology of an early-flowering species (Kobresia pygmaea), while it had no impact on the phenology of two mid-flowering species (Potentilla saundersiana and Potentilla cuneata). Compared to other low-altitude regions, plant phenology on the TP underwent greater alterations under eCO2, which supports our hypothesis that the growth of high-altitude plants is more sensitive to eCO2. Furthermore, we found that eCO2 significantly reduced the overlapping of flowering between contrasting plant species, mainly due to the phenological advancement of the K. pygmaea induced by eCO2. The observed advancement of the spring phenology in K. pygmaea under eCO2 was associated with increasing ecosystem water-use efficiency (WUE), thereby advancing its subsequent phenological development, such as budding and flowering. Our findings provide experimental evidence that atmospheric CO2 enrichment can accelerate plant growth processes in high-altitude regions, and suggest that large-scale model simulations should consider the effects of elevated atmospheric CO2 concentration on plant growth and phenology.

Disentangling the impact of climate change, human activities, vegetation dynamics and atmospheric CO2 concentration on soil water use efficiency in global karst landscapes

Soil Water Use Efficiency (SWUE), which quantifies the carbon gain against each unit of soil moisture depletion, represents an essential ecological parameter that delineates the carbon-water coupling within terrestrial ecosystems. However, the spatiotemporal dynamics of SWUE, its sensitivity to environmental variables, and the underlying driving mechanisms across various temporal scales in the global karst region are largely uncharted. This study utilized the sensitivity algorithm of partial least squares regression, partial differential equations, and elasticity coefficients to investigate the characteristics of SWUE variations across different climatic zones in the global karst region and their responsiveness to environmental variables. Moreover, the study quantified the individual contributions of climate variability, atmospheric carbon dioxide concentration, human activities, and vegetation changes to SWUE variations. The results indicated that SWUE across different climatic zones in the global karst region demonstrated an increasing trend from 2000 to 2018, with the most notable improvement observed in the humid zone. SWUE presented regular distribution and variation characteristics across different latitudinal zones at a monthly scale. The sensitivity of SWUE to precipitation was significantly higher compared to its responsiveness to other environmental factors. Additionally, the trend in SWUE's sensitivity to precipitation demonstrated the most significant change. The sensitivity of SWUE to various environmental factors and the trend of this sensitivity in the arid zone revealed significant variation compared to other climatic zones. Gross primary productivity and soil moisture were identified as the intrinsic factors influencing SWUE changes, contributing 16 % and − 84 %, respectively. Climate variability and human activities were identified as the primary exogenous factors contributing to the increase in SWUE, accounting for 76 % and 16 %, respectively. This study advances the understanding of carbon-water coupling in karst regions, providing significant insights into the ecological management of global karst environments amidst climate variations.

An Approach for Assessing Human Respiration CO2 Emissions Using Radiocarbon Measurements and Bottom‐Up Data Sets

AbstractCarbon dioxide (CO2) is a major greenhouse gas in the atmosphere and has large impacts on climate change. Its fossil fuel (CO2ff) and biogenic (CO2bio) sources are well investigated, while CO2 emissions from human respiration (CO2hr), a subset of CO2bio, have received less attention. Especially as a source of carbon emissions in densely populated megacities, the role of CO2hr emissions in the carbon cycles was largely neglected. Here we fully characterize the respiratory CO2 emission rates (CERs) of Chinese people for the first time. Using the example of the megacity Beijing in China, we estimate the CO2hr emissions and present a method for quantifying its fraction in the atmospheric CO2 based on radiocarbon (14C) measurements and inventory data sets. The results show that males and females have similar age trends in CERs, but the gender difference is significant, especially between the ages of 20 and 60, the average CERs was 33% higher for males than for females (P < 0.05). The CO2hr emissions were about 22.2 ± 0.6 kt CO2 per day, which was equivalent to 7.5% of daily CO2ff emissions in winter. The proportion is likely to be twice in summer due to the seasonal fluctuations of fossil fuel emissions. More importantly, the respiratory emissions could increase atmospheric CO2 concentration by about 2 ppm, accounting for 14% ± 6% of average CO2bio concentration in winter. This study highlights the importance of human respiration in carbon emissions in megacities and has implications for a better understanding of the regional carbon budget.

Ice sheet and precession controlled subarctic Pacific productivity and upwelling over the last 550,000 years

The polar oceans play a vital role in regulating atmospheric CO2 concentrations (pCO2) during the Pleistocene glacial cycles. However, despite being the largest modern reservoir of respired carbon, the impact of the subarctic Pacific remains poorly understood due to limited records. Here, we present high-resolution, 230Th-normalized export productivity records from the subarctic northwestern Pacific covering the last five glacial cycles. Our records display pronounced, glacial-interglacial cyclicity superimposed with precessional-driven variability, with warm interglacial climate and high boreal summer insolation providing favorable conditions to sustain upwelling of nutrient-rich subsurface waters and hence increased export productivity. Our transient model simulations consistently show that ice sheets and to a lesser degree, precession are the main drivers that control the strength and latitudinal position of the westerlies. Enhanced upwelling of nutrient/carbon-rich water caused by the intensification and poleward migration of the northern westerlies during warmer climate intervals would have led to the release of previously sequestered CO2 from the subarctic Pacific to the atmosphere. Our results also highlight the significant role of the subarctic Pacific in modulating pCO2 changes during the Pleistocene climate cycles, especially on precession timescale ( ~ 20 kyr).

Dependency of the impacts of geoengineering on the stratospheric sulfur injection strategy – Part 2: How changes in the hydrological cycle depend on the injection rate and model used

Abstract. This is the second of two papers in which we study the dependency of the impacts of stratospheric sulfur injections on the model and injection strategy used. Here, aerosol optical properties from simulated stratospheric aerosol injections using two aerosol models (modal scheme M7 and sectional scheme SALSA), as described in Part 1 (Laakso et al., 2022), are implemented consistently into the EC-Earth, MPI-ESM and CESM Earth system models (ESMs) to simulate the climate impacts of different injection rates ranging from 2 to 100 Tg(S) yr−1. Two sets of simulations were run with the three ESMs: (1) regression simulations, in which an abrupt change in CO2 concentration or stratospheric aerosols over pre-industrial conditions was applied to quantify global mean fast temperature-independent climate responses and quasi-linear dependence on temperature, and (2) equilibrium simulations, in which radiative forcing of aerosol injections with various magnitudes compensated for the corresponding radiative forcing of CO2 enhancement to study the dependence of precipitation on the injection magnitude. The latter also allow one to explore the regional climatic responses. Large differences in SALSA- and M7-simulated radiative forcing in Part 1 translated into large differences in the estimated surface temperature and precipitation changes in ESM simulations; for example, an injection rate of 20 Tg(S) yr−1 in CESM using M7-simulated aerosols led to only 2.2 K global mean cooling, while EC-Earth–SALSA combination produced a 5.2 K change. In equilibrium simulations, where aerosol injections were utilized to offset the radiative forcing caused by an atmospheric CO2 concentration of 500 ppm, the decrease in global mean precipitation varied among models, ranging from −0.7 % to −2.4 % compared with the pre-industrial climate. These precipitation changes can be explained by the fast precipitation response due to radiation changes caused by the stratospheric aerosols and CO2, as the global mean fast precipitation response is shown to be negatively correlated with global mean atmospheric absorption. Our study shows that estimating the impact of stratospheric aerosol injection on climate is not straightforward. This is because the simulated capability of the sulfate layer to reflect solar radiation and absorb long-wave radiation is sensitive to the injection rate as well as the aerosol model used to simulate the aerosol field. These findings emphasize the necessity for precise simulation of aerosol microphysics to accurately estimate the climate impacts of stratospheric sulfur intervention. This study also reveals gaps in our understanding and uncertainties that still exist related to these controversial techniques.

Poly(ionic liquid)-based aerogels for continuous-flow CO2 upcycling

The atmospheric concentration of CO2 is rising at an alarming pace, creating a pressing need for new and sustainable materials capable of capture and conversion. Poly(ionic liquid)s (PILs) are particularly effective catalysts for processes at or near atmospheric pressure. PILs industrial application poses challenges due to the low porosity of PIL, the limited batch conversion capacity, and the difficulties in reuse. To overcome these limitations, we herein propose the use of AEROPILs catalysts obtained from the integration of PILs in chitosan-based aerogels. These cost-effective highly porous materials have unique and tuneable porous properties making them not only ideal sustainable CO2 sorbents but also promising heterogeneous catalysts. While AEROPILs show moderate yields for CO2 conversion in batch mode, high catalytic activity was achieved when AEROPILs were used to catalyse the CO2 cycloaddition reaction to epoxides in packed-bed reactors operated under continuous flow. The catalytic activity and stability were maintained over 60 h without activity loss, and high productivity (space-time yield of 21.18 gprod h−1 L−1). This research reveals the pioneering use of AEROPILs to efficiently upcycle CO2 into cyclic carbonate under a continuous flow setup.

If Some Critical Regions Achieve Carbon Neutrality, How Will the Global Atmospheric CO2 Concentration Change?

Due to anthropogenic emissions, the global CO2 concentration increases at a rate of approximately 2 ppm per year. With over 130 countries and regions committing to carbon neutrality goals and continuously reducing anthropogenic CO2 emissions, understanding how atmospheric CO2 concentrations will change globally and in other regions has become an intriguing question. Examining different regions’ efforts to reduce anthropogenic CO2 emissions through atmospheric CO2 observations is also meaningful. We used prior and posterior fluxes to drive the TM5 model. The posterior fluxes were based on the China Carbon Monitoring, Verification and Support System for Global (CCMVS-G), which assimilated the atmospheric CO2 concentration data from ground-based observation and satellite observation. We found that the CO2 concentration obtained using the posterior fluxes was more in line with the actual situation. Then, we presented some experiments to estimate how global and regional CO2 concentrations would change if certain key regions and the whole world achieved net zero emissions of anthropogenic CO2. After removing carbon fluxes from China, North America, and Europe, global CO2 concentrations decreased by around 0.58 ppm, 0.22 ppm, and 0.10 ppm, respectively. The most significant decrease occurred in the regions where fluxes were removed, followed by other areas at the same latitude affected by westerly winds. This indicates that fossil fuel flux is the main factor affecting CO2 concentrations, and that meteorological-driven transportation also significantly impacts CO2 concentrations. Most importantly, using this method, it is possible to quantitatively estimate the impact of achieving carbon neutrality in one region on CO2 concentrations in local regions as well as globally.

Nutrient remobilization and C:N:P stoichiometry in response to elevated CO2 and low phosphorus availability in rice cultivars introgressed with and without Pup1

The continuously rising atmospheric CO2 concentration potentially increase plant growth through stimulating C metabolism; however, plant C:N:P stoichiometry in response to elevated CO2 (eCO2) under low P stress remains largely unknown. We investigated the combined effect of eCO2 and low phosphorus on growth, yield, C:N:P stoichiometry, and remobilization in rice cv. Kasalath (aus type), IR64 (a mega rice variety), and IR64-Pup1 (Pup1 QTL introgressed IR64). In response to eCO2 and low P, the C accumulation increased significantly (particularly at anthesis stage) while N and P concentration decreased leading to higher C:N and C:P ratios in all plant components (leaf, sheath, stem, and grain) than ambient CO2. The remobilization efficiencies of N and P were also reduced under low P with eCO2 as compared to control conditions. Among cultivars, the combined effect of eCO2 and low P was greater in IR64-Pup1 and produced higher biomass and grain yield as compared to IR64. However, IR64-Pup1 exhibited a lower N but higher P concentration than IR64, indicating that the Pup1 QTL improved P uptake but did not influence N uptake. Our study suggests that the P availability along with eCO2 would alter the C:N:P ratios due to their differential partitioning, thereby affecting growth and yield.

Evaluating the potential of iron-based interventions in methane reduction and climate mitigation

Keeping global surface temperatures below international climate targets will require substantial measures to control atmospheric CO2 and CH4 concentrations. Recent studies have focused on interventions to decrease CH4 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 CH4 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 CH4 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.

Orbital- and millennial-scale Asian winter monsoon variability across the Pliocene–Pleistocene glacial intensification

Intensification of northern hemisphere glaciation (iNHG), ~2.7 million years ago (Ma), led to establishment of the Pleistocene to present-day bipolar icehouse state. Here we document evolution of orbital- and millennial-scale Asian winter monsoon (AWM) variability across the iNHG using a palaeomagnetically dated centennial-resolution grain size record between 3.6 and 1.9 Ma from a previously undescribed loess-palaeosol/red clay section on the central Chinese Loess Plateau. We find that the late Pliocene–early Pleistocene AWM was characterized by combined 41-kyr and ~100-kyr cycles, in response to ice volume and atmospheric CO2 forcing. Northern hemisphere ice sheet expansion, which was accompanied by an atmospheric CO2 concentration decline, substantially increased glacial AWM intensity and its orbitally oscillating amplitudes across the iNHG. Superposed on orbital variability, we find that millennial AWM intensity fluctuations persisted during both the warmer (higher-CO2) late Pliocene and colder (lower-CO2) early Pleistocene, in response to both external astronomical forcing and internal climate dynamics.

Factors controlling long-term carbon sequestration in the paleo-Yellow River delta: Implications for future delta management

River deltas have contributed to the regulation of atmospheric CO2 concentrations throughout Earth's history, but the capacity and controlling factors for deltas to serve as permanent carbon sinks over the long term are unclear. To address this issue, we carried out a high-resolution assessment of carbon burial in a well-dated sediment core (BXZK13) from the paleo-Yellow River delta on the west coast of the Bohai Bay. We found that the sedimentary environments in core BXZK13 since the Late Pleistocene (∼84 k cal yr B.P.) were divided into seven depositional units. The apparent mass accumulation rate (AMAR) of total organic carbon (TOC) and total inorganic carbon (TIC) varied significantly between depositional units. The average rates were highest in delta front deposits (TOC: 135 g m−2 yr−1, TIC: 333 g m−2 yr−1). Notably, the rates of carbon accumulation were dominated by TIC. The differences in the characteristics of TIC in the borehole compare to those of carbonates in Yellow River sediments and the positive correlation between TIC and Fe suggested that authigenic carbonate contributed significantly to long-term carbon burial in the delta. The apparent sedimentation rate (ASR) dominated the variations of the carbon AMAR, and the high clay and Fe content in the sediment enhanced TOC preservation and authigenic carbonate precipitation. Low concentrations of TIC were associated with several cold events, and there was a positive correlation between the chemical index of alteration and TIC. The implication was that climate may have affected the dynamics of inorganic carbon burial by regulating authigenic carbonate precipitation. These results enable a more thorough understanding of the factors that control long-term carbon sequestration, which is critical for both management purposes as well as assessment of the role of deltas in past and future climate change.

Development of an autonomous on-site dissolved inorganic carbon analyzer using conductometric detection

BackgroundThe increase in anthropogenic CO2 concentrations in the Earth's atmosphere since the industrial revolution has resulted in an increased uptake of CO2 by the oceans, leading to ocean acidification. Dissolved Inorganic Carbon (DIC) is one of the key variables to characterize the seawater carbonate system. High quality DIC observations at a high spatial-temporal resolution is required to improve our understanding of the marine carbonate system. To meet the requirements, autonomous DIC analyzers are needed which offer a high sampling frequency, are cost-effective and have a low reagent and power consumption. ResultsWe present the development and validation of a novel analyzer for autonomous measurements of DIC in seawater using conductometric detection. The analyzer employs a gas diffusion sequential injection approach in a “Tube In A Tube” configuration that facilitates diffusion of gaseous CO2 from an acidified sample through a gas permeable membrane into a stream of an alkaline solution. The change in conductivity in the alkaline medium is proportional to the DIC concentration of the sample and is measured using a detection cell constructed of 4 hollow brass electrodes. Physical and chemical optimizations of the analyzer yielded a sampling frequency of 4 samples h−1 using sub mL reagent volumes for each measurement. Temperature and salinity effects on DIC measurements were mathematically corrected to increase accuracy. Analytical precision of ±4.9 μmol kg−1 and ±9.7 μmol kg−1 were achieved from measurements of a DIC reference material in the laboratory and during a field deployment in the southwest Baltic Sea, respectively. SignificanceThis study describes a simple, cost-effective, autonomous, on-site benchtop DIC analyzer capable of measuring DIC in seawater at a high temporal resolution as a step towards an underwater DIC sensor. The analyzer is able to measure a wide range of DIC concentrations in both fresh and marine waters. The achieved accuracy and precision offer an excellent opportunity to employ the analyzer for ocean acidification studies and CO2 leakage detection in the context of Carbon Capture and Storage operations.

Dual-Tuning Azole-Based Ionic Liquids for Reversible CO2 Capture from Ambient Air.

A strategy of tuning azole-based ionic liquids for reversible CO2 capture from ambient air was reported. Through tuning the basicity of anion as well as the type of cation, an ideal azole-based ionic liquid with both high CO2 capacity and excellent stability was synthesized, which exhibited a highest single-component isotherm uptake of 2.17 mmol/g at the atmospheric CO2 concentration of 0.4 mbar at 30 °C, even in the presence of water. The bound CO2 can be released by relatively mild heating of the IL-CO2 at 80 °C, which makes it promising for energy-efficient CO2 desorption and sorbent regeneration, leading to excellent reversibility. To the best of our knowledge, these azole-based ionic liquids are superior to other adsorbent materials for direct air capture due to their dual-tunable properties and high CO2 capture efficiency, offering a new prospect for efficient and reversible direct air capture technologies.

Breathing Planet Earth: Analysis of Keeling’s Data on CO2 and O2 with Respiratory Quotient (RQ), Part II: Energy-Based Global RQ and CO2 Budget

For breathing humans, the respiratory quotient (RQ = CO2 moles released/O2 mols consumed) ranges from 0.7 to 1.0. In Part I, the literature on the RQ was reviewed and Keeling’s data on atmospheric CO2 and O2 concentrations (1991–2018) were used in the estimation of the global RQ as 0.47. A new interpretation of RQGlob is provided in Part II by treating the planet as a “Hypothetical Biological system (HBS)”. The CO2 and O2 balance equations are adopted for estimating (i) energy-based RQGlob(En) and (ii) the CO2 distribution in GT/year and % of CO2 captured by the atmosphere, land, and ocean. The key findings are as follows: (i) The RQGlob(En) is estimated as 0.35 and is relatively constant from 1991 to 2020. The use of RQGlob(En) enables the estimation of CO2 added to the atmosphere from the knowledge of annual fossil fuel (FF) energy data; (ii) The RQ method for the CO2 budget is validated by comparing the annual CO2 distribution results with results from more detailed models; (iii) Explicit relations are presented for CO2 sink in the atmosphere, land, and ocean biomasses, and storage in ocean water from the knowledge of curve fit constants of Keeling’s curves and the RQ of FF and biomasses; (iv) The rate of global average temperature rise (0.27 °C/decade) is predicted using RQGlob,(En) and the annual energy release rate and compared with the literature data; and (v) Earth’s mass loss in GT and O2 in the atmosphere are predicted by extrapolating the curve fit to the year 3700. The effect of RQGlob and RQFF on the econometry and policy issues is briefly discussed.