Atmospheric particulate characterization by ToF-SIMS in an urban site in Beijing
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In this paper, we develop a framework and metrics for estimating the impact of emission sources on regulatory compliance and human health for applications in air quality planning and life cycle impact assessment (LCIA). Our framework is based on a pollutant's characterization factor (CF) and three new metrics: Available Regulatory Capacity for Incremental Emissions (ARCIE), Source CF Ratio, and Activity Health Impact (AHI) Ratio. ARCIE can be used to assess whether a receptor location has capacity to accommodate additional source emissions while complying with regulatory limits. We present CF as a midpoint indicator of health impacts per unit mass of emitted pollutant. Source CF Ratio enables comparison of potential new-source locations based on human health impacts. The AHI Ratio estimates the health impacts of a pollutant in relation to the utilization of the source for each unit of product or service. These metrics can be applied to any pollutant, energy source sector (e.g., agriculture, electricity), source type (point, line, area), and spatial modeling domain (nation, state, city, region). We demonstrate these metrics through a case study of fine particulate (PM 2.5 ) emissions from U.S. corn stover harvesting and local processing at various scales, representing steps in the biofuel production process. We model PM 2.5 formation in the atmosphere using a novel reduced-complexity chemical transport model called the Intervention Model for Air Pollution (InMAP). Through this case study, we present the first area-source PM 2.5 CFs that address the recommendations of several LCIA studies to establish spatially explicit CFs specific to an energy source sector or type. Overall, the framework developed in this work provides multiple new ways to consider the potential impacts of air emissions through spatially differentiated metrics.
Future climate change may worsen air quality in many regions. However, evaluations of this ‘climate penalty’ on air quality have typically not assessed the radiative effects of changes in short-lived aerosols. Additionally, China’s clean air goals will decrease pollutant emissions and aerosol loadings, with concomitant weakening of aerosol feedbacks. In this work, we assess how such weakened aerosol direct effects alter the estimates of air pollution and premature mortality in China attributable to mid-century climate change under Representative Concentration Pathway 4.5. We found that weakening aerosol direct effects cause boundary layer changes that facilitate diffusion. This reduces air-pollution exposure (~4% in fine particulate matter) and deaths (13,800 people per year), which largely offset the additional deaths caused by greenhouse gas-dominated warming. These results highlight the benefits of reduced pollutant emissions through weakening aerosol direct effects and underline the potential of pollution control measures to mitigate climate penalties locked in by greenhouse gas emissions.
Section 405(d) of the Clean Water Act requires the US Environmental Protection Agency to review sewage sludge regulations every two years to identify any additional pollutants that may occur in biosolids and to set regulations for pollutants identified in biosolids if sufficient scientific evidence shows they may harm human health or the environment. To date, EPA has conducted eight biennial reviews to identify chemical and microbial pollutants and three national sewage sludge surveys to identify pollutants and obtain concentration data for chemicals found in biosolids. Prior to 2021, there was inconsistent reporting of chemicals identified and EPA did not cumulatively track chemicals in biosolids. Through the efforts presented here, EPA produced a list of 726 chemicals and structure-based classes found in biosolids based on biennial reviews and national sewage sludge surveys. Summary statistics of concentration data are also reported for the 484 chemicals found in the three national sewage sludge surveys. The creation of the Biosolids List supports EPA in assessing the potential risk of chemical pollutants found in biosolids.
Severe haze is a major public health concern in China and India. Both countries rely heavily on coal for energy, and sulfur dioxide (SO 2 ) emitted from coal-fired power plants and industry is a major pollutant contributing to their air quality problems. Timely, accurate information on SO 2 sources is a required input to air quality models for pollution prediction and mitigation. However, such information has been difficult to obtain for these two countries, as fast-paced changes in economy and environmental regulations have often led to unforeseen emission changes. Here we use satellite observations to show that China and India are on opposite trajectories for sulfurous pollution. Since 2007, emissions in China have declined by 75% while those in India have increased by 50%. With these changes, India is now surpassing China as the world's largest emitter of anthropogenic SO 2 . This finding, not predicted by emission scenarios, suggests effective SO 2 control in China and lack thereof in India. Despite this, haze remains severe in China, indicating the importance of reducing emissions of other pollutants. In India, ~33 million people now live in areas with substantial SO 2 pollution. In conclusion, continued growth in emissions will adversely affect more people and further exacerbate morbidity and mortality.
To mitigate climate change, governments ranging from city to multi-national have adopted greenhouse gas (GHG) emissions reduction targets. While the location of GHG reductions does not affect their climate benefits, it can impact human health benefits associated with co-emitted pollutants. Here, an advanced modeling framework is used to explore how subnational level GHG targets influence air pollutant co-benefits from ground level ozone and fine particulate matter. Two carbon policy scenarios are analyzed, each reducing the same total amount of GHG emissions in the Northeast US: an economy-wide Cap and Trade (CAT) program reducing emissions from all sectors of the economy, and a Clean Energy Standard (CES) reducing emissions from the electricity sector only. Results suggest that a regional CES policy will cost about 10 times more than a CAT policy. Despite having the same regional targets in the Northeast, carbon leakage to non-capped regions varies between policies. Consequently, a regional CAT policy will result in national carbon reductions that are over six times greater than the carbon reduced by the CES in 2030. Monetized regional human health benefits of the CAT and CES policies are 844% and 185% of the costs of each policy, respectively. Benefits for both policies are thus estimated to exceed their costs in the Northeast US. The estimated value of human health co-benefits associated with air pollution reductions for the CES scenario is two times that of the CAT scenario. Implications: In this research, an advanced modeling framework is used to determine the potential impacts of regional carbon policies on air pollution co-benefits associated with ground level ozone and fine particulate matter. Study results show that spatially heterogeneous GHG policies have the potential to create areas of air pollution dis-benefit. It is also shown that monetized human health benefits within the area covered by policy may be larger than the model estimated cost of the policy. These findings are of particular interest both as U.S. states work to develop plans to meet state-level carbon emissions reduction targets set by the EPA through the Clean Power Plan, and in the absence of comprehensive national carbon policy.
This 3-year project has studied how aerosol pollution influences glaciated clouds. The tool applied has been an 'aerosol-cloud model'. It is a type of Cloud-System Resolving Model (CSRM) modified to include 2-moment bulk microphysics and 7 aerosol species, as described by Phillips et al. (2009, 2013). The study has been done by, first, improving the model and then performing sensitivity studies with validated simulations of a couple of observed cases from ARM. These are namely the Tropical Warm Pool International Cloud Experiment (TWP-ICE) over the tropical west Pacific and the Cloud and Land Surface Interaction Campaign (CLASIC) over Oklahoma. During the project, sensitivity tests with the model showed that in continental clouds, extra liquid aerosols (soluble aerosol material) from pollution inhibited warm rain processes for precipitation production. This promoted homogeneous freezing of cloud droplets and aerosols. Mass and number concentrations of cloud-ice particles were boosted. The mean sizes of cloud-ice particles were reduced by the pollution. Hence, the lifetime of glaciated clouds, especially ice-only clouds, was augmented due to inhibition of sedimentation and ice-ice aggregation. Latent heat released from extra homogeneous freezing invigorated convective updrafts, and raised their maximum cloud-tops, when aerosol pollution was included. In the particular cases simulated in the project, the aerosol indirect effect of glaciated clouds was twice than of (warm) water clouds. This was because glaciated clouds are higher in the troposphere than water clouds and have the first interaction with incoming solar radiation. Ice-only clouds caused solar cooling by becoming more extensive as a result of aerosol pollution. This 'lifetime indirect effect' of ice-only clouds was due to higher numbers of homogeneously nucleated ice crystals causing a reduction in their mean size, slowing the ice-crystal process of snow production and slowing sedimentation. In addition to the known indirect effects (glaciation, riming and thermodynamic), new indirect effects were discovered and quantified due to responses of sedimentation, aggregation and coalescence in glaciated clouds to changing aerosol conditions. In summary, the change in horizontal extent of the glaciated clouds ('lifetime indirect effects'), especially of ice-only clouds, was seen to be of higher importance in regulating aerosol indirect effects than changes in cloud properties ('cloud albedo indirect effects').
This 3-year project has studied how aerosol pollution influences glaciated clouds. The tool applied has been an 'aerosol-cloud model'. It is a type of Cloud-System Resolving Model (CSRM) modified to include 2-moment bulk microphysics and 7 aerosol species, as described by Phillips et al. (2009, 2013). The study has been done by, first, improving the model and then performing sensitivity studies with validated simulations of a couple of observed cases from ARM. These are namely the Tropical Warm Pool International Cloud Experiment (TWP-ICE) over the tropical west Pacific and the Cloud and Land Surface Interaction Campaign (CLASIC) over Oklahoma. During the project, sensitivity tests with the model showed that in continental clouds, extra liquid aerosols (soluble aerosol material) from pollution inhibited warm rain processes for precipitation production. This promoted homogeneous freezing of cloud droplets and aerosols. Mass and number concentrations of cloud-ice particles were boosted. The mean sizes of cloud-ice particles were reduced by the pollution. Hence, the lifetime of glaciated clouds, especially ice-only clouds, was augmented due to inhibition of sedimentation and ice-ice aggregation. Latent heat released from extra homogeneous freezing invigorated convective updrafts, and raised their maximum cloud-tops, when aerosol pollution was included. In the particular cases simulated in the project, the aerosol indirect effect of glaciated clouds was twice than of (warm) water clouds. This was because glaciated clouds are higher in the troposphere than water clouds and have the first interaction with incoming solar radiation. Ice-only clouds caused solar cooling by becoming more extensive as a result of aerosol pollution. This 'lifetime indirect effect' of ice-only clouds was due to higher numbers of homogeneously nucleated ice crystals causing a reduction in their mean size, slowing the ice-crystal process of snow production and slowing sedimentation. In addition to the known indirect effects (glaciation, riming and thermodynamic), new indirect effects were discovered and quantified due to responses of sedimentation, aggregation and coalescence in glaciated clouds to changing aerosol conditions. In summary, the change in horizontal extent of the glaciated clouds ('lifetime indirect effects'), especially of ice-only clouds, was seen to be of higher importance in regulating aerosol indirect effects than changes in cloud properties ('cloud albedo indirect effects').
Substantial energy is used to condition the air that enters California homes through leaks in the building envelope and ductwork - typically about a third of all heating and cooling. Reducing this through air sealing is essential to California achieving zero energy homes. However, this outdoor air also dilutes pollutants emitted inside homes and contributes to a healthy indoor environment and acceptable indoor air quality (IAQ). To address this IAQ issue, California’s Title 24 Building Standards have required mechanical ventilation in new homes since 2008. This report presents a comprehensive study of the impacts of these requirements in recently constructed homes with natural gas appliances. The study included a survey about satisfaction and activities that impact IAQ; a field study of homes built to 2008 or later; and simulations assessing how various ventilation rates would impact chronic exposures to an indoor emitted pollutant as air tightness improves in California. The report focuses on the field study; the webbased survey and simulation elements are described in appendices. The field study characterized 70 homes built between 2011 and 2017. Each home was monitored over roughly one week with the dwelling unit mechanical ventilation system operating and windows closed. Pollutant measurements included time-resolved fine particulate matter (PM 2.5 ) indoors and outdoors, and formaldehyde, nitrogen dioxide (NO 2 ), and carbon dioxide (CO 2 ) indoors. Time-integrated measurements were made for formaldehyde, NO 2 and nitrogen oxides (NO X ) indoors and outdoors at all homes. Activity monitoring devices were installed on the cooktop, range hood and other exhaust fans, and the heating and cooling system. The field study found that most homes met most ventilation requirements and the dwelling unit ventilation fans on average moved 50% more airflow than the minimum specified in Title 24. Air pollutant concentrations were similar or lower than those reported in a study of recent construction California new homes conducted in 2007-08. Notably, the median formaldehyde level was 38% lower than in the prior study. Measured concentrations were below health guidelines for most pollutants, indicating that IAQ is acceptable in new California homes when dwelling unit mechanical ventilation is used. However, the dwelling unit mechanical ventilation fans were only operating in one quarter of the homes when first visited and the control switches in many homes did not have informative labels as required by the standards. Corrective action needs to be taken to improve labeling and controls for ventilation systems.
Vehicle emission is a major source of air pollution. A significant number of deaths is associated with air pollution. The existing vehicle emission monitoring system is unable to mitigate the pollution properly. Real-time pollution measurement is necessary to address the problem more precisely. The purpose of this project is to develop novel Vehicle Emission Monitoring Applications (VEMA) using the real-time measurement of pollutants from a vehicle tailpipe where exhaust gases enter the environment. As a part of the project, 2 technologies have been used for exhaust gas monitoring. First, an off-the-shelf exhaust gas monitoring prototype has been acquired. Second, a brand new platform was developed using off-the-shelf components. The project focused on predictive application for smart mobility and for large large fleet companies and enterprises. A data collection methodology was developed and tested by collecting close to 20 hours of data within Washington State under varying speeds, altitudes, road conditions etc. An approach for data curation was also used and finally, a simple Machine Learning was used for recognizing patterns between inputs such as vehicle speed and altitude and output such as NOx emission from vehicle exhaust pipe.
The Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) Experiment was carried out in the environs of Manaus, Brazil, in the central region of the Amazon basin for 2 years from 1 January 2014 through 31 December 2015. The experiment focused on the complex interactions among vegetation, atmospheric chemistry, and aerosol production on the one hand and their connections to aerosols, clouds, and precipitation on the other. The objective was to understand and quantify these linked processes, first under natural conditions to obtain a baseline and second when altered by the effects of human activities. To this end, the pollution plume from the Manaus metropolis, superimposed on the background conditions of the central Amazon basin, served as a natural laboratory. The present paper, as the introduction to the special issue of GoAmazon2014/5, presents the context and motivation of the GoAmazon2014/5 Experiment. The nine research sites, including the characteristics and instrumentation of each site, are presented. The sites range from time point zero (T0) upwind of the pollution, to T1 in the midst of the pollution, to T2 just downwind of the pollution, to T3 furthest downwind of the pollution (70 km). In addition to the ground sites, a low-altitude G-159 Gulfstream I (G-1) observed the atmospheric boundary layer and low clouds, and a high-altitude Gulfstream G550 (HALO) operated in the free troposphere. During the 2-year experiment, two Intensive Operating Periods (IOP1 and IOP2) also took place that included additional specialized research instrumentation at the ground sites as well as flights of the two aircraft. GoAmazon2014/5 IOP1 was carried out from 1 February to 31 March 2014 in the wet season. GoAmazon2014/5 IOP2 was conducted from 15 August to 15 October 2014 in the dry season. In addition, the G-1 aircraft flew during both IOP1 and IOP2, and the HALO aircraft flew during IOP2. In the context of the Amazon basin, the two IOPs also correspond to the clean and biomass burning seasons, respectively. The Manaus plume is present year-round, and it is transported by prevailing northeasterly and easterly winds in the wet and dry seasons, respectively. This introduction also organizes information relevant to many papers in the special issue. Information is provided on the vehicle fleet, power plants, and industrial activities of Manaus. The mesoscale and synoptic meteorologies relevant to the two IOPs are presented. Regional and long-range transport of emissions during the two IOPs is discussed based on satellite observations across South America and Africa. Fire locations throughout the airshed are detailed. In conjunction with the context and motivation of GoAmazon2014/5 as presented in this introduction, research articles including thematic overview articles are anticipated in this special issue to describe the detailed results and findings of the GoAmazon2014/5 Experiment.
Motivated by recent discussions concerning differences of convective dynamics in polluted and pristine environments, the so-called convective invigoration in particular, this paper provides an analysis of factors affecting convective updraft buoyancy, such as the in-cloud supersaturation, condensate and precipitation loading, and entrainment. We use the deep convective period from simulations of daytime convection development over land discussed in our previous publications. An entraining parcel framework is used in the theoretical analysis. We show that for the specific case considered here, finite (positive) supersaturation noticeably reduces pseudo-adiabatic parcel buoyancy and cumulative convective available potential energy (cCAPE) in the lower troposphere. This comes from keeping a small fraction of the water vapor in a supersaturated state and thus reducing the latent heating. Such a lower-tropospheric impact is comparable to the effects of condensate loading and entrainment in the idealized parcel framework. For the entire tropospheric depth, loading and entrainment have a much more significant impact on the total CAPE. For the cloud model results, we compare ensemble simulations applying either a bulk microphysics scheme with saturation adjustment or a more comprehensive double-moment scheme with supersaturation prediction. We compare deep convective updraft velocities, buoyancies, and supersaturations from all ensembles. In agreement with the parcel analysis, the saturation-adjustment scheme provides noticeably stronger updrafts in the lower troposphere. For the simulations predicting supersaturation, there are small differences between pristine and polluted conditions below the freezing level that are difficult to explain by standard analysis of the in-cloud buoyancy components. By applying the piggybacking technique, we show that the lower-tropospheric buoyancy differences between pristine and polluted simulations come from a combination of temperature (i.e., latent heating) and condensate loading differences that work together to make polluted buoyancies and updraft velocities slightly larger when compared to their pristine analogues. Overall, the effects are rather small and contradict previous claims of a significant invigoration of deep convection in polluted environments.
Retrievals of total column NO 2 (TCNO 2 ) are compared for 14 sites from the Ozone Measuring Instrument (OMI using OMNO2-NASA v3.1) on the AURA satellite and from multiple ground-based PANDORA spectrometer instruments making direct-sun measurements. While OMI accurately provides the daily global distribution of retrieved TCNO 2 , OMI almost always underestimates the local amount of TCNO 2 by 50 % to 100 % in polluted areas, while occasionally the daily OMI value exceeds that measured by PANDORA at very clean sites. Compared to local ground-based or aircraft measurements, OMI cannot resolve spatially variable TCNO 2 pollution within a city or urban areas, which makes it less suitable for air quality assessments related to human health. In addition to systematic underestimates in polluted areas, OMI's selected 13:30 Equator crossing timepolar orbit causes it to miss the frequently much higher values of TCNO 2 that occur before or after the OMI overpass time. Six discussed Northern Hemisphere PANDORA sites have multi-year data records (Busan,Seoul, Washington DC, Waterflow, New Mexico, Boulder, Colorado, and Mauna Loa),and one site in the Southern Hemisphere (Buenos Aires, Argentina). The first four of these sites and Buenos Aires frequently have high TCNO 2 (TCNO 2 > 0.5 DU). Eight additional sites have shorter-term data records in the US and South Korea. One of these is a 1-year data record from a highly polluted site at City College in New York City with pollution levels comparable to Seoul, South Korea. OMI-estimated air mass factor, surface reflectivity, and the OMI 24 km × 13 km FOV (field of view)are three factors that can cause OMI to underestimate TCNO 2 . Because of the local inhomogeneity of NO x emissions, the large OMI FOV is the most likely factor for consistent underestimates when comparing OMI TCNO 2 to retrievals from the small PANDORA effective FOV (measured in m 2 ) calculated from the solar diameter of 0.5°.
The available techniques were examined in the field of remote sensing (including aerial photography, infrared detection, radar, etc.) and applications to a number of problems in the wide field of public health determined. The specific areas of public health examined included: air pollution, water pollution, communicable disease, and the combined problems of urban growth and the effect of disasters on human communities. The assessment of the possible applications of remote sensing to these problems was made primarily by examination of the available literature in each field, and by interviews with health authorities, physicists, biologists, and other interested workers. Three types of programs employing remote sensors were outlined in the air pollution field: (1) proving ability of sensors to monitor pollutants at three levels of interest - point source, ambient levels in cities, and global patterns; (2) detection of effects of pollutants on the environment at local and global levels; and (3) routine monitoring.
An instrumented aircraft was used to study the chemical and transport properties of air pollution in two major urban centers in California and to survey certain aspects of air pollution within this state. State-of-the-art measurement techniques and sampling procedures are discussed. It is found that meteorological transport mechanisms are better portrayed by vertical pollutant profiles. Airborne measurements define the nature of the mixing layer for atmospheric pollutants. Results show that the pollutants are found to be concentrated in distinct layers up to at least 18,000 feet and the O3 buildup occurring in advected air masses is a result of a continuous photochemical aging of air mass.
The transfer of LANDSAT remote sensing technology from the research sector to user operational applications requires demonstration of the utility and accuracy of LANDSAT data in solving real problems. This report describes such a demonstration project in the area of water resources, specifically the estimation of non-point source pollutant loads. Non-point source pollutants were estimated from land cover data from LANDSAT images. Classification accuracies for three small watersheds were above 95%. Land cover was converted to pollutant loads for a fourth watershed through the use of coefficients relating significant pollutants to land use and storm runoff volume. These data were input into a simulator model which simulated runoff from average rainfall. The result was the estimation of monthly expected pollutant loads for the 17 subbasins comprising the Magothy watershed.
During the Atlantic Stratocumulus Transition Experiment (ASTEX) in June 1992, two descents in cloud-free regions allowed comparison of the change in aerosol optical depth as determined by an onboard total-direct-diffuse radiometer (TDDR) to the change calculated from measured size-resolved aerosol microphysics and chemistry. Both profiles included a pollution haze from Europe but the second also included the effect of a Saharan dust layer above the haze. The separate contributions of supermicrometer (coarse) and submicrometer (fine) aerosol were determined and thermal analysis of the pollution haze indicated that the fine aerosol was composed primarily of a sulfate/water mixture with a refractory soot-like core. The soot core increased the calculated extinction by about 10% in the most polluted drier layer relative to a pure sulfate aerosol but had significantly less effect at higher humidities. A 3 km descent through a boundary layer air mass dominated by pollutant aerosol with relative humidities (RH) 10-77% yielded a close agreement between the measured and calculated aerosol optical depths (550 nm) of 0.160 (+/- 0.07) and 0. 157 (+/- 0.034) respectively. During descent the aerosol mass scattering coefficient per unit sulfate mass varied from about 5 to 16 m(exp 2)/g and primarily dependent upon ambient RH. However, the total scattering coefficient per total fine mass was far less variable at about 4+/- 0.7 m(exp 2)/g. A subsequent descent through a Saharan dust layer located above the pollution aerosol layer revealed that both layers contributed similarly to aerosol optical depth. The scattering per unit mass of the coarse aged dust was estimated at 1.1 +/- 0.2 m(exp 2)/g. The large difference (50%) in measured and calculated optical depth for the dust layer exceeded measurements.
Flight 10 of NASA's Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) extended southwest of Lajes, Azores. A variety of chemical signatures were encountered. These signatures are examined in detail, relating them to meteorological data from a high resolution numerical model having horizontal grid spacing of 30 and 90 km and 26 vertical levels. The meteorological output at hourly intervals is used to create backward trajectories from the locations of the chemical signatures. Four major categories of chemical signatures are discussed-stratospheric, lightning, continental pollution, and a transition layer. The strong stratospheric signal is encountered just south of the Azores in a region of depressed tropopause height. Three chemical signatures at different altitudes in the upper troposphere are attributed to lightning. Backward trajectories arriving at locations of these signatures are related to locations of cloud-to-ground lightning. Results show that the trajectories pass through regions of lightning 1-2 days earlier over the eastern Gulf of Mexico and off the southeast coast of the United States. The lowest leg of the flight exhibits a chemical signature consistent with continental pollution. Trajectories arriving at this signature are found to pass over the highly populated Northeast Corridor of the United States. Surface based pollution apparently is lofted to the altitudes of the trajectories by convective clouds along the East Coast that did not contain lightning. Finally, a chemical transition layer is described. Its chemical signature is intermediate to those of lightning and continental pollution. Trajectories arriving in this layer pass between the trajectories of the lightning and pollution signatures. Thus, they probably are impacted by both sources.