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1.
Proc Natl Acad Sci U S A ; 115(20): 5099-5104, 2018 05 15.
Artigo em Inglês | MEDLINE | ID: mdl-29712822

RESUMO

Ground and satellite observations show that air pollution regulations in the United States (US) have resulted in substantial reductions in emissions and corresponding improvements in air quality over the last several decades. However, large uncertainties remain in evaluating how recent regulations affect different emission sectors and pollutant trends. Here we show a significant slowdown in decreasing US emissions of nitrogen oxides (NO x ) and carbon monoxide (CO) for 2011-2015 using satellite and surface measurements. This observed slowdown in emission reductions is significantly different from the trend expected using US Environmental Protection Agency (EPA) bottom-up inventories and impedes compliance with local and federal agency air-quality goals. We find that the difference between observations and EPA's NO x emission estimates could be explained by: (i) growing relative contributions of industrial, area, and off-road sources, (ii) decreasing relative contributions of on-road gasoline, and (iii) slower than expected decreases in on-road diesel emissions.


Assuntos
Poluentes Atmosféricos/análise , Poluição do Ar/análise , Monóxido de Carbono/análise , Monitoramento Ambiental/normas , Óxidos de Nitrogênio/análise , Material Particulado/análise , Emissões de Veículos/análise , Gasolina , Humanos , Estados Unidos
2.
Environ Sci Technol ; 54(11): 6518-6529, 2020 06 02.
Artigo em Inglês | MEDLINE | ID: mdl-32348127

RESUMO

Urban ozone (O3) formation can be limited by NOx, VOCs, or both, complicating the design of effective O3 abatement plans. A satellite-retrieved ratio of formaldehyde to NO2 (HCHO/NO2), developed from theory and modeling, has previously been used to indicate O3 formation chemistry. Here, we connect this space-based indicator to spatiotemporal variations in O3 recorded by on-the-ground monitors over major U.S. cities. High-O3 events vary nonlinearly with OMI HCHO and NO2, and the transition from VOC-limited to NOx-limited O3 formation regimes occurs at higher HCHO/NO2 value (3 to 4) than previously determined from models, with slight intercity variations. To extend satellite records back to 1996, we develop an approach to harmonize observations from GOME and SCIAMACHY that accounts for differences in spatial resolution and overpass time. Two-decade (1996-2016) multisatellite HCHO/NO2 captures the timing and location of the transition from VOC-limited to NOx-limited O3 production regimes in major U.S. cities, which aligns with the observed long-term changes in urban-rural gradient of O3 and the reversal of O3 weekend effect. Our findings suggest promise for applying space-based HCHO/NO2 to interpret local O3 chemistry, particularly with the new-generation satellite instruments that offer finer spatial and temporal resolution.


Assuntos
Poluentes Atmosféricos , Ozônio , Compostos Orgânicos Voláteis , Poluentes Atmosféricos/análise , Cidades , Monitoramento Ambiental , Ozônio/análise , Compostos Orgânicos Voláteis/análise
3.
Environ Sci Technol ; 50(1): 331-7, 2016 Jan 05.
Artigo em Inglês | MEDLINE | ID: mdl-26642237

RESUMO

A decade (2005-2014) of observations from the Ozone Monitoring Instrument (OMI) were used to examine trends in nitrogen dioxide (NO2) and sulfur dioxide (SO2) over a large region of western Canada and the northern United States, with a focus on the Canadian oil sands. In the oil sands, primarily over an area of intensive surface mining, NO2 tropospheric vertical column densities (VCDs) are seen to be increasing by as much as 10%/year, with the location of the largest trends in a newly developing NO2 "lobe" well removed from surface monitoring stations. SO2 VCDs in the oil sands have remained approximately constant. The only other significant increase in the region was seen in NO2 over Bakken gas fields in North Dakota which showed increases of up to 5%/yr. By contrast, other locations in the region show substantial declines in both pollutants, providing strong evidence to the efficacy of environmental pollution control measures implemented by both nations. The OMI-derived trends were found to be consistent with those from the Canadian surface monitoring network, although in the case of SO2, it was necessary to apply a correction in order to remove the residual signal from volcanic eruptions present in the OMI data.


Assuntos
Poluentes Atmosféricos/análise , Poluição do Ar/análise , Monitoramento Ambiental/métodos , Dióxido de Nitrogênio/análise , Campos de Petróleo e Gás , Dióxido de Enxofre/análise , Canadá , North Dakota
4.
Sci Adv ; 9(29): eadg7429, 2023 07 21.
Artigo em Inglês | MEDLINE | ID: mdl-37478188

RESUMO

Response actions to the coronavirus disease 2019 perturbed economies and carbon dioxide (CO2) emissions. The Omicron variant that emerged in 2022 caused more substantial infections than in 2020 and 2021 but it has not yet been ascertained whether Omicron interrupted the temporary post-2021 rebound of CO2 emissions. Here, using satellite nitrogen dioxide observations combined with atmospheric inversion, we show a larger decline in China's CO2 emissions between January and April 2022 than in those months during the first wave of 2020. China's CO2 emissions are estimated to have decreased by 15% (equivalent to -244.3 million metric tons of CO2) during the 2022 lockdown, greater than the 9% reduction during the 2020 lockdown. Omicron affected most of the populated and industrial provinces in 2022, hindering China's CO2 emissions rebound starting from 2021. China's emission variations agreed with downstream CO2 concentration changes, indicating a potential to monitor CO2 emissions by integrating satellite and ground measurements.


Assuntos
COVID-19 , Dióxido de Carbono , Humanos , Dióxido de Carbono/análise , COVID-19/epidemiologia , SARS-CoV-2 , Controle de Doenças Transmissíveis , China
5.
Atmos Chem Phys ; 21(14): 11133-11160, 2021 Jul 23.
Artigo em Inglês | MEDLINE | ID: mdl-35949546

RESUMO

Nitrogen oxides (NO x =NO+NO2) play a crucial role in the formation of ozone and secondary inorganic and organic aerosols, thus affecting human health, global radiation budget, and climate. The diurnal and spatial variations in NO2 are functions of emissions, advection, deposition, vertical mixing, and chemistry. Their observations, therefore, provide useful constraints in our understanding of these factors. We employ a Regional chEmical and trAnsport model (REAM) to analyze the observed temporal (diurnal cycles) and spatial distributions of NO2 concentrations and tropospheric vertical column densities (TVCDs) using aircraft in situ measurements and surface EPA Air Quality System (AQS) observations as well as the measurements of TVCDs by satellite instruments (OMI: the Ozone Monitoring Instrument; GOME-2A: Global Ozone Monitoring Experiment - 2A), ground-based Pandora, and the Airborne Compact Atmospheric Mapper (ACAM) instrument in July 2011 during the DISCOVER-AQ campaign over the Baltimore-Washington region. The model simulations at 36 and 4 km resolutions are in reasonably good agreement with the regional mean temporospatial NO2 observations in the daytime. However, we find significant overestimations (underestimations) of model-simulated NO2 (O3) surface concentrations during night-time, which can be mitigated by enhancing nocturnal vertical mixing in the model. Another discrepancy is that Pandora-measured NO2 TVCDs show much less variation in the late afternoon than simulated in the model. The higher-resolution 4 km simulations tend to show larger biases compared to the observations due largely to the larger spatial variations in NO x emissions in the model when the model spatial resolution is increased from 36 to 4 km. OMI, GOME-2A, and the high-resolution aircraft ACAM observations show a more dispersed distribution of NO2 vertical column densities (VCDs) and lower VCDs in urban regions than corresponding 36 and 4 km model simulations, likely reflecting the spatial distribution bias of NO x emissions in the National Emissions Inventory (NEI) 2011.

6.
Artigo em Inglês | MEDLINE | ID: mdl-30297473

RESUMO

The tropical carbon balance dominates year-to-year variations in the CO2 exchange with the atmosphere through photosynthesis, respiration and fires. Because of its high correlation with gross primary productivity (GPP), observations of sun-induced fluorescence (SIF) are of great interest. We developed a new remotely sensed SIF product with improved signal-to-noise in the tropics, and use it here to quantify the impact of the 2015/2016 El Niño Amazon drought. We find that SIF was strongly suppressed over areas with anomalously high temperatures and decreased levels of water in the soil. SIF went below its climatological range starting from the end of the 2015 dry season (October) and returned to normal levels by February 2016 when atmospheric conditions returned to normal, but well before the end of anomalously low precipitation that persisted through June 2016. Impacts were not uniform across the Amazon basin, with the eastern part experiencing much larger (10-15%) SIF reductions than the western part of the basin (2-5%). We estimate the integrated loss of GPP relative to eight previous years to be 0.34-0.48 PgC in the three-month period October-November-December 2015.This article is part of a discussion meeting issue 'The impact of the 2015/2016 El Niño on the terrestrial tropical carbon cycle: patterns, mechanisms and implications'.


Assuntos
El Niño Oscilação Sul , Fluorescência , Tecnologia de Sensoriamento Remoto/métodos , Luz Solar , Árvores/fisiologia , Brasil , Secas , Florestas
7.
J Geophys Res Atmos ; 122(19): 10-461, 2017 Oct 16.
Artigo em Inglês | MEDLINE | ID: mdl-29682438

RESUMO

Determining effective strategies for mitigating surface ozone (O3) pollution requires knowledge of the relative ambient concentrations of its precursors, NO x , and VOCs. The space-based tropospheric column ratio of formaldehyde to NO2 (FNR) has been used as an indicator to identify NO x -limited versus NO x -saturated O3 formation regimes. Quantitative use of this indicator ratio is subject to three major uncertainties: (1) the split between NO x -limited and NO x -saturated conditions may shift in space and time, (2) the ratio of the vertically integrated column may not represent the near-surface environment, and (3) satellite products contain errors. We use the GEOS-Chem global chemical transport model to evaluate the quantitative utility of FNR observed from the Ozone Monitoring Instrument over three northern midlatitude source regions. We find that FNR in the model surface layer is a robust predictor of the simulated near-surface O3 production regime. Extending this surface-based predictor to a column-based FNR requires accounting for differences in the HCHO and NO2 vertical profiles. We compare four combinations of two OMI HCHO and NO2 retrievals with modeled FNR. The spatial and temporal correlations between the modeled and satellite-derived FNR vary with the choice of NO2 product, while the mean offset depends on the choice of HCHO product. Space-based FNR indicates that the spring transition to NO x -limited regimes has shifted at least a month earlier over major cities (e.g., New York, London, and Seoul) between 2005 and 2015. This increase in NO x sensitivity implies that NO x emission controls will improve O3 air quality more now than it would have a decade ago.

8.
Sci Rep ; 2: 265, 2012.
Artigo em Inglês | MEDLINE | ID: mdl-22355777

RESUMO

Fuel combustion is a significant source of numerous air pollutants, which reduce local air quality, and affect global tropospheric chemistry. Satellite observations of nitrogen dioxide, emitted by combustion processes, allow for robust monitoring of atmospheric concentrations at high spatial resolution on continental scales. Here we evaluate changes in tropospheric NO(2) concentrations over Europe between 2004 and 2010. We isolate long-term (timescales greater than one year) variability in the daily NO(2) observations from the Ozone Monitoring Instrument (OMI) using a spectral analysis. In 2010, we find substantial reductions in NO(2) concentrations of at least 20% throughout Europe. These reductions are as much the result of temporary reductions prompted by the 2008-2009 global economic recession, as of European NO(x) emission controls. Our results demonstrate that realistic concentration pathways of NO(2) do not follow simple linear trends, but reflect a compilation of environmental policy and economic activity.

9.
Science ; 333(6050): 1737-9, 2011 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-21940891

RESUMO

Megacities are immense sources of air pollutants, with large impacts on air quality and climate. However, emission inventories in many of them still are highly uncertain, particularly in developing countries. Satellite observations allow top-down estimates of emissions to be made for nitrogen oxides (NO(x) = NO + NO(2)), but require poorly quantified a priori information on the NO(x) lifetime. We present a method for the simultaneous determination of megacity NO(x) emissions and lifetimes from satellite measurements by analyzing the downwind patterns of NO(2) separately for different wind conditions. Daytime lifetimes are ~4 hours at low and mid-latitudes, but ~8 hours in wintertime for Moscow. The derived NO(x) emissions are generally in good agreement with existing emission inventories, but are higher by a factor of 3 for the Saudi Arabian capital Riyadh.

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