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1.
Proc Natl Acad Sci U S A ; 121(6): e2309333121, 2024 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-38289951

RESUMO

We present improved estimates of air-sea CO2 exchange over three latitude bands of the Southern Ocean using atmospheric CO2 measurements from global airborne campaigns and an atmospheric 4-box inverse model based on a mass-indexed isentropic coordinate (Mθe). These flux estimates show two features not clearly resolved in previous estimates based on inverting surface CO2 measurements: a weak winter-time outgassing in the polar region and a sharp phase transition of the seasonal flux cycles between polar/subpolar and subtropical regions. The estimates suggest much stronger summer-time uptake in the polar/subpolar regions than estimates derived through neural-network interpolation of pCO2 data obtained with profiling floats but somewhat weaker uptake than a recent study by Long et al. [Science 374, 1275-1280 (2021)], who used the same airborne data and multiple atmospheric transport models (ATMs) to constrain surface fluxes. Our study also uses moist static energy (MSE) budgets from reanalyses to show that most ATMs tend to have excessive diabatic mixing (transport across moist isentrope, θe, or Mθe surfaces) at high southern latitudes in the austral summer, which leads to biases in estimates of air-sea CO2 exchange. Furthermore, we show that the MSE-based constraint is consistent with an independent constraint on atmospheric mixing based on combining airborne and surface CO2 observations.

2.
Nature ; 586(7828): 248-256, 2020 10.
Artigo em Inglês | MEDLINE | ID: mdl-33028999

RESUMO

Nitrous oxide (N2O), like carbon dioxide, is a long-lived greenhouse gas that accumulates in the atmosphere. Over the past 150 years, increasing atmospheric N2O concentrations have contributed to stratospheric ozone depletion1 and climate change2, with the current rate of increase estimated at 2 per cent per decade. Existing national inventories do not provide a full picture of N2O emissions, owing to their omission of natural sources and limitations in methodology for attributing anthropogenic sources. Here we present a global N2O inventory that incorporates both natural and anthropogenic sources and accounts for the interaction between nitrogen additions and the biochemical processes that control N2O emissions. We use bottom-up (inventory, statistical extrapolation of flux measurements, process-based land and ocean modelling) and top-down (atmospheric inversion) approaches to provide a comprehensive quantification of global N2O sources and sinks resulting from 21 natural and human sectors between 1980 and 2016. Global N2O emissions were 17.0 (minimum-maximum estimates: 12.2-23.5) teragrams of nitrogen per year (bottom-up) and 16.9 (15.9-17.7) teragrams of nitrogen per year (top-down) between 2007 and 2016. Global human-induced emissions, which are dominated by nitrogen additions to croplands, increased by 30% over the past four decades to 7.3 (4.2-11.4) teragrams of nitrogen per year. This increase was mainly responsible for the growth in the atmospheric burden. Our findings point to growing N2O emissions in emerging economies-particularly Brazil, China and India. Analysis of process-based model estimates reveals an emerging N2O-climate feedback resulting from interactions between nitrogen additions and climate change. The recent growth in N2O emissions exceeds some of the highest projected emission scenarios3,4, underscoring the urgency to mitigate N2O emissions.


Assuntos
Óxido Nitroso/análise , Óxido Nitroso/metabolismo , Agricultura , Atmosfera/química , Produtos Agrícolas/metabolismo , Atividades Humanas , Internacionalidade , Nitrogênio/análise , Nitrogênio/metabolismo
3.
Glob Chang Biol ; 29(15): 4298-4312, 2023 08.
Artigo em Inglês | MEDLINE | ID: mdl-37190869

RESUMO

The recent rise in atmospheric methane (CH4 ) concentrations accelerates climate change and offsets mitigation efforts. Although wetlands are the largest natural CH4 source, estimates of global wetland CH4 emissions vary widely among approaches taken by bottom-up (BU) process-based biogeochemical models and top-down (TD) atmospheric inversion methods. Here, we integrate in situ measurements, multi-model ensembles, and a machine learning upscaling product into the International Land Model Benchmarking system to examine the relationship between wetland CH4 emission estimates and model performance. We find that using better-performing models identified by observational constraints reduces the spread of wetland CH4 emission estimates by 62% and 39% for BU- and TD-based approaches, respectively. However, global BU and TD CH4 emission estimate discrepancies increased by about 15% (from 31 to 36 TgCH4 year-1 ) when the top 20% models were used, although we consider this result moderately uncertain given the unevenly distributed global observations. Our analyses demonstrate that model performance ranking is subject to benchmark selection due to large inter-site variability, highlighting the importance of expanding coverage of benchmark sites to diverse environmental conditions. We encourage future development of wetland CH4 models to move beyond static benchmarking and focus on evaluating site-specific and ecosystem-specific variabilities inferred from observations.


Assuntos
Ecossistema , Áreas Alagadas , Metano/análise , Mudança Climática , Previsões , Dióxido de Carbono
4.
Glob Chang Biol ; 28(1): 182-200, 2022 01.
Artigo em Inglês | MEDLINE | ID: mdl-34553464

RESUMO

The ongoing development of the Global Carbon Project (GCP) global methane (CH4 ) budget shows a continuation of increasing CH4 emissions and CH4 accumulation in the atmosphere during 2000-2017. Here, we decompose the global budget into 19 regions (18 land and 1 oceanic) and five key source sectors to spatially attribute the observed global trends. A comparison of top-down (TD) (atmospheric and transport model-based) and bottom-up (BU) (inventory- and process model-based) CH4 emission estimates demonstrates robust temporal trends with CH4 emissions increasing in 16 of the 19 regions. Five regions-China, Southeast Asia, USA, South Asia, and Brazil-account for >40% of the global total emissions (their anthropogenic and natural sources together totaling >270 Tg CH4  yr-1 in 2008-2017). Two of these regions, China and South Asia, emit predominantly anthropogenic emissions (>75%) and together emit more than 25% of global anthropogenic emissions. China and the Middle East show the largest increases in total emission rates over the 2000 to 2017 period with regional emissions increasing by >20%. In contrast, Europe and Korea and Japan show a steady decline in CH4 emission rates, with total emissions decreasing by ~10% between 2000 and 2017. Coal mining, waste (predominantly solid waste disposal) and livestock (especially enteric fermentation) are dominant drivers of observed emissions increases while declines appear driven by a combination of waste and fossil emission reductions. As such, together these sectors present the greatest risks of further increasing the atmospheric CH4 burden and the greatest opportunities for greenhouse gas abatement.


Assuntos
Atmosfera , Metano , Animais , China , Gado , Metano/análise , Oceanos e Mares
5.
Glob Chang Biol ; 26(3): 1068-1084, 2020 03.
Artigo em Inglês | MEDLINE | ID: mdl-31828914

RESUMO

Robust estimates of CO2 budget, CO2 exchanged between the atmosphere and terrestrial biosphere, are necessary to better understand the role of the terrestrial biosphere in mitigating anthropogenic CO2 emissions. Over the past decade, this field of research has advanced through understanding of the differences and similarities of two fundamentally different approaches: "top-down" atmospheric inversions and "bottom-up" biosphere models. Since the first studies were undertaken, these approaches have shown an increasing level of agreement, but disagreements in some regions still persist, in part because they do not estimate the same quantity of atmosphere-biosphere CO2 exchange. Here, we conducted a thorough comparison of CO2 budgets at multiple scales and from multiple methods to assess the current state of the science in estimating CO2 budgets. Our set of atmospheric inversions and biosphere models, which were adjusted for a consistent flux definition, showed a high level of agreement for global and hemispheric CO2 budgets in the 2000s. Regionally, improved agreement in CO2 budgets was notable for North America and Southeast Asia. However, large gaps between the two methods remained in East Asia and South America. In other regions, Europe, boreal Asia, Africa, South Asia, and Oceania, it was difficult to determine whether those regions act as a net sink or source because of the large spread in estimates from atmospheric inversions. These results highlight two research directions to improve the robustness of CO2 budgets: (a) to increase representation of processes in biosphere models that could contribute to fill the budget gaps, such as forest regrowth and forest degradation; and (b) to reduce sink-source compensation between regions (dipoles) in atmospheric inversion so that their estimates become more comparable. Advancements on both research areas will increase the level of agreement between the top-down and bottom-up approaches and yield more robust knowledge of regional CO2 budgets.


Assuntos
Dióxido de Carbono , Ecossistema , África , Ásia , Europa (Continente) , América do Norte , América do Sul
6.
Phys Chem Chem Phys ; 19(38): 26330-26345, 2017 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-28936513

RESUMO

Novel approaches to boost quantum dot solar cell (QDSC) efficiencies are in demand. Herein, three strategies are used: (i) a hydrothermally synthesized TiO2-multiwalled carbon nanotube (MWCNT) composite instead of conventional TiO2, (ii) a counter electrode (CE) that has not been applied to QDSCs until now, namely, tin sulfide (SnS) nanoparticles (NPs) coated over a conductive carbon (C)-fabric, and (iii) a quasi-solid-state gel electrolyte composed of S2-, an inert polymer and TiO2 nanoparticles as opposed to a polysulfide solution based hole transport layer. MWCNTs by virtue of their high electrical conductivity and suitably positioned Fermi level (below the conduction bands of TiO2 and PbS) allow fast photogenerated electron injection into the external circuit, and this is confirmed by a higher efficiency of 6.3% achieved for a TiO2-MWCNT/PbS/ZnS based (champion) cell, compared to the corresponding TiO2/PbS/ZnS based cell (4.45%). Nanoscale current map analysis of TiO2 and TiO2-MWCNTs reveals the presence of narrowly spaced highly conducting domains in the latter, which equips it with an average current carrying capability greater by a few orders of magnitude. Electron transport and recombination resistances are lower and higher respectively for the TiO2-MWCNT/PbS/ZnS cell relative to the TiO2/PbS/ZnS cell, thus leading to a high performance cell. The efficacy of SnS/C-fabric as a CE is confirmed from the higher efficiency achieved in cells with this CE compared to the C-fabric based cells. Lower charge transfer and diffusional resistances, slower photovoltage decay, high electrical conductance and lower redox potential impart high catalytic activity to the SnS/C-fabric assembly for sulfide reduction and thus endow the TiO2-MWCNT/PbS/ZnS cell with a high open circuit voltage (0.9 V) and a large short circuit current density (∼20 mA cm-2). This study attempts to unravel how simple strategies can amplify QDSC performances.

7.
Proc Natl Acad Sci U S A ; 111(49): 17379-84, 2014 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-25422438

RESUMO

HCFC-22 (CHClF2) and HFC-134a (CH2FCF3) are two major gases currently used worldwide in domestic and commercial refrigeration and air conditioning. HCFC-22 contributes to stratospheric ozone depletion, and both species are potent greenhouse gases. In this work, we study in situ observations of HCFC-22 and HFC-134a taken from research aircraft over the Pacific Ocean in a 3-y span [HIaper-Pole-to-Pole Observations (HIPPO) 2009-2011] and combine these data with long-term ground observations from global surface sites [National Oceanic and Atmospheric Administration (NOAA) and Advanced Global Atmospheric Gases Experiment (AGAGE) networks]. We find the global annual emissions of HCFC-22 and HFC-134a have increased substantially over the past two decades. Emissions of HFC-134a are consistently higher compared with the United Nations Framework Convention on Climate Change (UNFCCC) inventory since 2000, by 60% more in recent years (2009-2012). Apart from these decadal emission constraints, we also quantify recent seasonal emission patterns showing that summertime emissions of HCFC-22 and HFC-134a are two to three times higher than wintertime emissions. This unforeseen large seasonal variation indicates that unaccounted mechanisms controlling refrigerant gas emissions are missing in the existing inventory estimates. Possible mechanisms enhancing refrigerant losses in summer are (i) higher vapor pressure in the sealed compartment of the system at summer high temperatures and (ii) more frequent use and service of refrigerators and air conditioners in summer months. Our results suggest that engineering (e.g., better temperature/vibration-resistant system sealing and new system design of more compact/efficient components) and regulatory (e.g., reinforcing system service regulations) steps to improve containment of these gases from working devices could effectively reduce their release to the atmosphere.

8.
J Nanosci Nanotechnol ; 16(3): 2668-76, 2016 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-27455687

RESUMO

A novel design of a laboratory built axially rotating collector (ARC) having capability to align electrospun nanofibers have been described. A detailed morphological comparison of such nanofibers orientation and their geometry is done using scanning electron microscopy (SEM). For comparison various polymeric solutions were electrospun on conventional static collector as well as ARC. The average diameter of polyvinyl alcohol (PVA) nanofibers was found to be 250 nm while polycaprolactone (PCL) nanofibers were found to be within a range of 600-800 nm. Conducting nanoparticles such as graphene and multi-walled carbon nanotubes (MWNTs) mixed with polymer solutions shown to have a significant influence on the overall geometry of these nanofibers and their diameter distribution. It is evident from the SEM analysis that both graphene and MWNTs in polymer solution play a crucial role in achieving a uniform diameter of nanofibers. Lastly, the formation of the aligned nanofibers using ARC has been mathematically modeled and the electromagnetic field governing the process has been simulated.


Assuntos
Nanofibras , Microscopia Eletrônica de Varredura , Poliésteres/química , Álcool de Polivinil/química
9.
Environ Toxicol ; 31(9): 1091-102, 2016 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-25689286

RESUMO

With their unique structure and physicochemical properties, single\-walled carbon nanotubes (SWCNTs) have many potential new applications in medicine and industry. However, there is lack of detailed information concerning their impact on human health and the environment. The aim of this study was to assess the effects, after intraperitoneal injection of functionalized SWCNTs (f-SWCNT) on the induction of reactive oxygen species (ROS), frequency of structural chromosomal aberrations (SCA), frequency of micronuclei induction, mitotic index, and DNA damage in Swiss-Webster mice. Three doses of f-SWCNTs (0.25, 0.5, and 0.75 mg/kg) and two controls (negative and positive) were administered to mice, once a day for 5 days. Bone marrow and peripheral blood samples were collected 24 h after the last treatment following standard protocols. F-SWCNT exposure significantly enhanced ROS, increased (p < 0.05) the number of SCA and the frequency of micronucleated cells, increased DNA damage, and decreased the mitotic index in exposed groups compared to negative control. The scientific findings reported here suggest that purified f-SWCNT have the potential to induce oxidative stress mediated genotoxicity in Swiss-Webster mice at higher level of exposure. Further characterization of their systemic toxicity, genotoxicity, and carcinogenicity is also essential. © 2015 Wiley Periodicals, Inc. Environ Toxicol 31: 1091-1102, 2016.


Assuntos
Células da Medula Óssea/efeitos dos fármacos , Aberrações Cromossômicas/efeitos dos fármacos , Nanotubos de Carbono/toxicidade , Animais , Células da Medula Óssea/citologia , Células da Medula Óssea/metabolismo , Células Cultivadas , Ensaio Cometa , Dano ao DNA/efeitos dos fármacos , Injeções Intraperitoneais , Masculino , Camundongos , Microscopia Eletrônica de Varredura , Nanotubos de Carbono/ultraestrutura , Estresse Oxidativo/efeitos dos fármacos , Espécies Reativas de Oxigênio/metabolismo
10.
Environ Eng Sci ; 31(6): 288-299, 2014 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-24963270

RESUMO

A potential ion-exchange material was developed from poly(acrylonitrile) fibers that were prepared by electrospinning followed by alkaline hydrolysis (to convert the nitrile group to the carboxylate functional group). Characterization studies performed on this material using X-ray photoelectron spectroscopy, scanning electron microscopy, Fourier-Transform infra-red spectroscopy, and ion chromatography confirmed the presence of ion-exchange functional group (carboxylate). Optimum hydrolysis conditions resulted in an ion-exchange capacity of 2.39 meq/g. Ion-exchange fibers were used in a packed-bed column to selectively remove heavy-metal cation from the background of a benign, competing cation at a much higher concentration. The material can be efficiently regenerated and used for multiple cycles of exhaustion and regeneration.

11.
Sci Total Environ ; 921: 171226, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38402969

RESUMO

The present study investigated the effects of land use/land cover (LU/LC) changes on atmospheric carbon dioxide (CO2) and methane (CH4) concentrations over the sub-urban region of India (Shadnagar) using continuous decadal CO2 and CH4in-situ data measured by the greenhouse gas analyser (GGA). Data was collected from 2013 to 2022 at a 1 Hz frequency. Analysis of the current study indicates that during pre-monsoon, the seasonal maximum of CO2 was 409.91 ± 9.26 ppm (µ ± 1σ), while the minimum during monsoon was about 401.64 ± 7.13 ppm. Post-monsoon has a high seasonal mean CH4 concentration of 2.08 ± 0.06 ppm, while monsoon has a low seasonal mean CH4 concentration of 1.88 ± 0.03 ppm. The primary classes, such as forest, crop, and built-up, were considered to estimate the effect of LU/LC changes on atmospheric CO2 and CH4 concentrations. Between 2005 and 2021, the study's results show that the built-up area at radii of 10 km, 20 km, and 50 km increased by 0.17 %, 0.10 %, and 0.4 %, respectively. While other LU/LC categories declined by 30 %, agriculture areas increased by 30 % on average. As a result, the CO2 and CH4 concentrations at the study site are increased by 6 % (26 ppm) and 6.5 % (140 ppb), respectively. The present study utilised the fire-based carbon emissions data from the Global Fire Emissions Database (GFED) to understand the impact on atmospheric CO2 and CH4. Analysis of the present work investigated the influence of transported airmass on CO2 and CH4 during the pre-monsoon and post-monsoon seasons using the HYSPLIT trajectories and found emissions were from the northwest, southeast, and northeast of the study site. Further, in-situ CO2 and CH4 records are compared against the MIROC4-ACTM simulation, and strong agreement was found with bias of 1.80 ppm and 0.98 ppb for CO2 and CH4, respectively.

12.
Prog Earth Planet Sci ; 10(1): 10, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36879643

RESUMO

We developed a near-real-time estimation method for temporal changes in fossil fuel CO2 (FFCO2) emissions from China for 3 months [January, February, March (JFM)] based on atmospheric CO2 and CH4 observations on Hateruma Island (HAT, 24.06° N, 123.81° E) and Yonaguni Island (YON, 24.47° N, 123.01° E), Japan. These two remote islands are in the downwind region of continental East Asia during winter because of the East Asian monsoon. Previous studies have revealed that monthly averages of synoptic-scale variability ratios of atmospheric CO2 and CH4 (ΔCO2/ΔCH4) observed at HAT and YON in JFM are sensitive to changes in continental emissions. From the analysis based on an atmospheric transport model with all components of CO2 and CH4 fluxes, we found that the ΔCO2/ΔCH4 ratio was linearly related to the FFCO2/CH4 emission ratio in China because calculating the variability ratio canceled out the transport influences. Using the simulated linear relationship, we converted the observed ΔCO2/ΔCH4 ratios into FFCO2/CH4 emission ratios in China. The change rates of the emission ratios for 2020-2022 were calculated relative to those for the preceding 9-year period (2011-2019), during which relatively stable ΔCO2/ΔCH4 ratios were observed. These changes in the emission ratios can be read as FFCO2 emission changes under the assumption of no interannual variations in CH4 emissions and biospheric CO2 fluxes for JFM. The resulting average changes in the FFCO2 emissions in January, February, and March 2020 were 17 ± 8%, - 36 ± 7%, and - 12 ± 8%, respectively, (- 10 ± 9% for JFM overall) relative to 2011-2019. These results were generally consistent with previous estimates. The emission changes for January, February, and March were 18 ± 8%, - 2 ± 10%, and 29 ± 12%, respectively, in 2021 (15 ± 10% for JFM overall) and 20 ± 9%, - 3 ± 10%, and - 10 ± 9%, respectively, in 2022 (2 ± 9% for JFM overall). These results suggest that the FFCO2 emissions from China rebounded to the normal level or set a new high record in early 2021 after a reduction during the COVID-19 lockdown. In addition, the estimated reduction in March 2022 might be attributed to the influence of a new wave of COVID-19 infections in Shanghai. Supplementary Information: The online version contains supplementary material available at 10.1186/s40645-023-00542-6.

13.
Sci Rep ; 13(1): 13201, 2023 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-37580480

RESUMO

Exposure to particulate matter less than 2.5 µm in diameter (PM2.5) is a cause of concern in cities and major emission regions of northern India. An intensive field campaign involving the states of Punjab, Haryana and Delhi national capital region (NCR) was conducted in 2022 using 29 Compact and Useful PM2.5 Instrument with Gas sensors (CUPI-Gs). Continuous observations show that the PM2.5 in the region increased gradually from < 60 µg m-3 in 6-10 October to up to 500 µg m-3 on 5-9 November, which subsequently decreased to about 100 µg m-3 in 20-30 November. Two distinct plumes of PM2.5 over 500 µg m-3 are tracked from crop residue burning in Punjab to Delhi NCR on 2-3 November and 10-11 November with delays of 1 and 3 days, respectively. Experimental campaign demonstrates the advantages of source region observations to link agricultural waste burning and air pollution at local to regional scales.

14.
Sci Total Environ ; 842: 156721, 2022 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-35716737

RESUMO

Methane (CH4) is a potent greenhouse gas and also plays a significant role in tropospheric chemistry. High-frequency (sub-hourly) measurements of CH4 and carbon isotopic ratio (δ13CH4) have been conducted at Pune (18.53°N, 73.80°E), an urban environment in India, during 2018-2020. High CH4 concentrations were observed, with a mean of 2100 ± 196 ppb (1844-2749 ppb), relative to marine background concentrations. The δ13CH4 varied between -45.11 and -50.03 ‰ for the entire study period with an average of -47.41 ± 0.94 ‰. The diurnal variability of CH4 typically showed maximum values in the morning (08:00-09:00 local time) and minimum in the afternoon (15:00 local time). The deepest diurnal amplitude of ~500 ppb was observed during winter (December-February), which was reduced to less than half, ~200 ppb, during the summer (March-May). CH4 concentration at Pune showed a strong seasonality (470 ppb), much higher than that at Mauna Loa, Hawaii. On the other hand, δ13CH4 records did not show distinct seasonality at Pune. The δ13CH4 values revealed that the significant sources of CH4 in Pune were from the waste sector (enhanced during the monsoon season; signature of depleted δ13CH4), followed by the natural gas sector with a signature of enriched δ13CH4. Our analysis of Covid-19 lockdown (April to May 2020) effect on the CH4 variability showed no signal in the CH4 variability; however, the isotopic analysis indicated a transient shift in the CH4 source to the waste sector (early summer of 2020).


Assuntos
Poluentes Atmosféricos , COVID-19 , Poluentes Atmosféricos/análise , Controle de Doenças Transmissíveis , Monitoramento Ambiental , Humanos , Índia , Metano/análise , Gás Natural/análise
15.
J Geophys Res Atmos ; 127(13): e2021JD035892, 2022 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-35864859

RESUMO

Long-term measurements at the Mauna Loa Observatory (MLO) show that the CO2 seasonal cycle amplitude (SCA) increased from 1959 to 2019 at an overall rate of 0.22  ±  0.034 ppm decade-1 while also varying on interannual to decadal time scales. These SCA changes are a signature of changes in land ecological CO2 fluxes as well as shifting winds. Simulations with the TM3 tracer transport model and CO2 fluxes from the Jena CarboScope CO2 Inversion suggest that shifting winds alone have contributed to a decrease in SCA of -0.10  ±  0.022 ppm decade-1 from 1959 to 2019, partly offsetting the observed long-term SCA increase associated with enhanced ecosystem net primary production. According to these simulations and MIROC-ACTM simulations, the shorter-term variability of MLO SCA is nearly equally driven by varying ecological CO2 fluxes (49%) and varying winds (51%). We also show that the MLO SCA is strongly correlated with the Pacific Decadal Oscillation (PDO) due to varying winds, as well as with a closely related wind index (U-PDO). Since 1980, 44% of the wind-driven SCA decrease has been tied to a secular trend in the U-PDO, which is associated with a progressive weakening of westerly winds at 700 mbar over the central Pacific from 20°N to 40°N. Similar impacts of varying winds on the SCA are seen in simulations at other low-latitude Pacific stations, illustrating the difficulty of constraining trend and variability of land CO2 fluxes using observations from low latitudes due to the complexity of circulation changes.

16.
Sci Total Environ ; 819: 153114, 2022 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-35041945

RESUMO

Carbon dioxide (CO2) and methane (CH4) are the most important greenhouse gases (GHGs) due to their significant role in anthropogenic global climate change. The spatio-temporal variations of their concentration are characterized by the terrestrial biosphere, seasonal weather patterns and anthropogenic emissions. Hence, to understand the variability in regional surface GHG fluxes, high precision GHGs measurements were initiated by the National Remote Sensing Center (NRSC) of India. We report continuous CO2 and CH4measurements during 2014 to 2017 for the first time from Shadnagar, a suburban site in India. Annual mean CO2 and CH4 concentrations are 399.56 ± 5.46 ppm and 1.929 ± 0.09 ppm, respectively, for 2017. After the strong El Niño of 2015-2016, an abnormal rise in CO2 growth rate of 5.5 ppm year-1 was observed in 2017 at the study site, compared to 3.03 ppm year-1 at Mauna Loa. Thus, the repercussion of the El Niño effect diminishes the net uptake by the terrestrial biosphere accompanied by increased soil respiration. Seasonal tracer to tracer correlation between CO2 and CH4 was also analyzed to characterize the possible source-sink relationship between the species. We compared CO2 and CH4 concentrations to simulations from an atmospheric chemistry transport model (ACTM). The seasonal phases of CH4 were well captured by the ACTM, whereas the seasonal cycle amplitude of CO2 was underestimated by about 30%.


Assuntos
Dióxido de Carbono , Gases de Efeito Estufa , Dióxido de Carbono/análise , Gases de Efeito Estufa/análise , Metano/análise , Óxido Nitroso/análise , Estações do Ano , Solo
17.
Natl Sci Rev ; 9(5): nwab200, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-35547958

RESUMO

Atmospheric methane (CH4) concentrations have shown a puzzling resumption in growth since 2007 following a period of stabilization from 2000 to 2006. Multiple hypotheses have been proposed to explain the temporal variations in CH4 growth, and attribute the rise of atmospheric CH4 either to increases in emissions from fossil fuel activities, agriculture and natural wetlands, or to a decrease in the atmospheric chemical sink. Here, we use a comprehensive ensemble of CH4 source estimates and isotopic δ13C-CH4 source signature data to show that the resumption of CH4 growth is most likely due to increased anthropogenic emissions. Our emission scenarios that have the fewest biases with respect to isotopic composition suggest that the agriculture, landfill and waste sectors were responsible for 53 ± 13% of the renewed growth over the period 2007-2017 compared to 2000-2006; industrial fossil fuel sources explained an additional 34 ± 24%, and wetland sources contributed the least at 13 ± 9%. The hypothesis that a large increase in emissions from natural wetlands drove the decrease in atmospheric δ13C-CH4 values cannot be reconciled with current process-based wetland CH4 models. This finding suggests the need for increased wetland measurements to better understand the contemporary and future role of wetlands in the rise of atmospheric methane and climate feedback. Our findings highlight the predominant role of anthropogenic activities in driving the growth of atmospheric CH4 concentrations.

18.
Nat Commun ; 13(1): 5626, 2022 09 26.
Artigo em Inglês | MEDLINE | ID: mdl-36163194

RESUMO

Warming of northern high latitude regions (NHL, > 50 °N) has increased both photosynthesis and respiration which results in considerable uncertainty regarding the net carbon dioxide (CO2) balance of NHL ecosystems. Using estimates constrained from atmospheric observations from 1980 to 2017, we find that the increasing trends of net CO2 uptake in the early-growing season are of similar magnitude across the tree cover gradient in the NHL. However, the trend of respiratory CO2 loss during late-growing season increases significantly with increasing tree cover, offsetting a larger fraction of photosynthetic CO2 uptake, and thus resulting in a slower rate of increasing annual net CO2 uptake in areas with higher tree cover, especially in central and southern boreal forest regions. The magnitude of this seasonal compensation effect explains the difference in net CO2 uptake trends along the NHL vegetation- permafrost gradient. Such seasonal compensation dynamics are not captured by dynamic global vegetation models, which simulate weaker respiration control on carbon exchange during the late-growing season, and thus calls into question projections of increasing net CO2 uptake as high latitude ecosystems respond to warming climate conditions.


Assuntos
Dióxido de Carbono , Pergelissolo , Ciclo do Carbono , Ecossistema , Estações do Ano
19.
Sci Data ; 8(1): 2, 2021 01 07.
Artigo em Inglês | MEDLINE | ID: mdl-33414478

RESUMO

Quantification of CO2 fluxes at the Earth's surface is required to evaluate the causes and drivers of observed increases in atmospheric CO2 concentrations. Atmospheric inversion models disaggregate observed variations in atmospheric CO2 concentration to variability in CO2 emissions and sinks. They require prior constraints fossil CO2 emissions. Here we describe GCP-GridFED (version 2019.1), a gridded fossil emissions dataset that is consistent with the national CO2 emissions reported by the Global Carbon Project (GCP). GCP-GridFEDv2019.1 provides monthly fossil CO2 emissions estimates for the period 1959-2018 at a spatial resolution of 0.1°. Estimates are provided separately for oil, coal and natural gas, for mixed international bunker fuels, and for the calcination of limestone during cement production. GCP-GridFED also includes gridded estimates of O2 uptake based on oxidative ratios for oil, coal and natural gas. It will be updated annually and made available for atmospheric inversions contributing to GCP global carbon budget assessments, thus aligning the prior constraints on top-down fossil CO2 emissions with the bottom-up estimates compiled by the GCP.

20.
Sci Rep ; 11(1): 9800, 2021 05 07.
Artigo em Inglês | MEDLINE | ID: mdl-33963208

RESUMO

COVID-19 related restrictions lowered particulate matter and trace gas concentrations across cities around the world, providing a natural opportunity to study effects of anthropogenic activities on emissions of air pollutants. In this paper, the impact of sudden suspension of human activities on air pollution was analyzed by studying the change in satellite retrieved NO2 concentrations and top-down NOx emission over the urban and rural areas around Delhi. NO2 was chosen for being the most indicative of emission intensity due to its short lifetime of the order of a few hours in the planetary boundary layer. We present a robust temporal comparison of Ozone Monitoring Instrument (OMI) retrieved NO2 column density during the lockdown with the counterfactual baseline concentrations, extrapolated from the long-term trend and seasonal cycle components of NO2 using observations during 2015 to 2019. NO2 concentration in the urban area of Delhi experienced an anomalous relative change ranging from 60.0% decline during the Phase 1 of lockdown (March 25-April 13, 2020) to 3.4% during the post-lockdown Phase 5. In contrast, we find no substantial reduction in NO2 concentrations over the rural areas. To segregate the impact of the lockdown from the meteorology, weekly top-down NOx emissions were estimated from high-resolution TROPOspheric Monitoring Instrument (TROPOMI) retrieved NO2 by accounting for horizontal advection derived from the steady state continuity equation. NOx emissions from urban Delhi and power plants exhibited a mean decline of 72.2% and 53.4% respectively in Phase 1 compared to the pre-lockdown business-as-usual phase. Emission estimates over urban areas and power-plants showed a good correlation with activity reports, suggesting the applicability of this approach for studying emission changes. A higher anomaly in emission estimates suggests that comparison of only concentration change, without accounting for the dynamical and photochemical conditions, may mislead evaluation of lockdown impact. Our results shall also have a broader impact for optimizing bottom-up emission inventories.


Assuntos
Poluentes Atmosféricos/análise , Poluição do Ar/análise , COVID-19/prevenção & controle , Controle de Doenças Transmissíveis , Monitoramento Ambiental , Dióxido de Nitrogênio/análise , COVID-19/epidemiologia , Cidades , Humanos , Índia/epidemiologia , Óxidos de Nitrogênio/análise , SARS-CoV-2/isolamento & purificação
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