Qirui Zhong

Quantification of Global Primary Emissions of PM2.5, PM10, and TSP from Combustion and Industrial Process Sources

Emission quantification of primary particulate matter (PM) is essential for assessment of its related climate and health impacts. To reduce uncertainty associated with global emissions of PM2.5, PM10, and TSP, we compiled data with high spatial (0.1° × 0.1°) and sectorial (77 primary sources) resolutions for 2007 based on a newly released global fuel data product (PKU-FUEL-2007) and an emission factor database. Our estimates for developing countries are higher than those previously reported. Spatial bias associated with large countries could be reduced by using subnational fuel consumption data. Additionally, we looked at temporal trends from 1960 to 2009 at country-scale resolution. Although total emissions are still increasing in developing countries, their intensities in terms of gross domestic production or energy consumption have decreased. PM emitted in developed countries is finer owing to a larger contribution from nonindustrial sources and use of abatement technologies. In contrast, countries like China, with strong industry emissions and limited abatement facilities, emit coarser PM. The health impacts of PM are intensified in hotspots and cities owing to covariance of sources and receptors. Although urbanization reduces the per person emission, overall health impacts related to these emissions are heightened because of aggregation effects.

Concentrations and origins of nitro-polycyclic aromatic hydrocarbons and oxy-polycyclic aromatic hydrocarbons in ambient air in urban and rural areas in northern China

Twelve nitro-PAHs (nPAHs) and four oxy-PAHs (oPAHs) were measured in air samples for 12 months at 18 sites in urban settings, rural villages, or rural fields in northern China. The nPAH concentrations were higher in urban areas (1.3 ± 1.3 ng/m(3)), and nPAH/parent PAH ratios were higher (suggesting important contributions from motor vehicles and secondary formation) in urban sites than in rural villages. oPAHs are primarily emitted from solid fuel combustion and motor vehicles, and similar oPAH concentrations were found in urban areas (23 ± 20 ng/m(3)) and rural villages (29 ± 24 ng/m(3)). The high numbers of motor vehicles in Beijing and intensive industrial activity in Taiyuan and Dezhou caused higher nPAH concentrations. No spatial trend in oPAH concentrations was found in the rural villages, because similar oPAH mixtures are emitted from solild fuel combustion. The nPAH and oPAH concentrations were higher in the winter, and correlated with residential energy consumption and precipitation.

Daily variations of size-segregated ambient particulate matter in Beijing

Daily, size-segregated particulate matter (PM) samples were collected at Peking University from March 2012 to April 2013. Seventeen indoor air samples were also collected over this period. Winter PM concentrations decreased compared with those reported a decade ago, but summer PM concentrations increased over the same time period. Increasing summer PM concentrations likely resulted from a shift in the major source of PM from primary coal burning to vehicle-associated secondary particle formation. A multiple regression model explained 62% of daily PM concentration variations, and wind direction was the most important factor controlling PM concentrations. Severe pollution was often associated with southeasterly winds, while westerly and northwesterly winds brought relatively clean air. Temperature, precipitation and relative humidity also affected PM concentrations. PM concentrations indoors were generally lower than, but significantly correlated with ambient concentrations. Indoor PM concentrations were also affected by wind speed and temperature.

Improvement of a Global High-Resolution Ammonia Emission Inventory for Combustion and Industrial Sources with New Data from the Residential and Transportation Sectors

There is increasing evidence indicating the critical role of ammonia (NH3) in the formation of secondary aerosols. Therefore, high quality NH3 emission inventory is important for modeling particulate matter in the atmosphere. Unfortunately, without directly measured emission factors (EFs) in developing countries, using data from developed countries could result in an underestimation of these emissions. A series of newly reported EFs for China provide an opportunity to update the NH3 emission inventory. In addition, a recently released fuel consumption data product has allowed for a multisource, high-resolution inventory to be assembled. In this study, an improved global NH3 emission inventory for combustion and industrial sources with high sectorial (70 sources), spatial (0.1° × 0.1°), and temporal (monthly) resolutions was compiled for the years 1960 to 2013. The estimated emissions from transportation (1.59 Tg) sectors in 2010 was 2.2 times higher than those of previous reports. The spatial variation of the emissions was associated with population, gross domestic production, and temperature. Unlike other major air pollutants, NH3 emissions continue to increase, even in developed countries, which is likely caused by an increased use of biomass fuel in the residential sector. The emissions density of NH3 in urban areas is an order of magnitude higher than in rural areas.

Exposure and health impact evaluation based on simultaneous measurement of indoor and ambient PM2.5 in Haidian, Beijing.

Because people spend most of their time indoors, the characterization of indoor air quality is important for exposure assessment. Unfortunately, indoor air data are scarce, leading to a major data gap in risk assessment. In this study, PM2.5 concentrations in both indoor and outdoor air were simultaneously measured using on-line particulate counters in 13 households in Haidian, Beijing for both heating and non-heating seasons. A bimodal distribution of PM2.5 concentrations suggests rapid transitions between polluted and non-polluted situations. The PM2.5 concentrations in indoor and outdoor air varied synchronously, with the indoor variation lagging. The lag time in the heating season was longer than that in the non-heating season. The particle sizes in indoor air were smaller than those in ambient air in the heating season and vice versa in the non-heating season. PM2.5 concentrations in indoor air were generally lower than those in ambient air except when ambient concentrations dropped sharply to very low levels or there were internal emissions from cooking or other activities. The effectiveness of an air cleaner to reduce indoor PM2.5 concentrations was demonstrated. Non-linear regression models were developed to predict indoor air PM2.5 concentrations based on ambient data with lag time incorporated. The models were applied to estimate the overall population exposure to PM2.5 and the health consequences in Haidian. The health impacts would be significantly overestimated without the indoor exposure being taken into consideration, and this bias would increase as the ambient air quality improved in the future.

Urbanization-induced population migration has reduced ambient PM2.5 concentrations in China

Population migration has upgraded the direct energy consumption with remarkable benefits on air quality and health in China. Direct residential and transportation energy consumption (RTC) contributes significantly to ambient fine particulate matter with a diameter smaller than 2.5 μm (PM2.5) in China. During massive rural-urban migration, population and pollutant emissions from RTC have evolved in terms of magnitude and geographic distribution, which was thought to worsen PM2.5 levels in cities but has not been quantitatively addressed. We quantify the temporal trends and spatial patterns of migration to cities and evaluate their associated pollutant emissions from RTC and subsequent health impact from 1980 to 2030. We show that, despite increased urban RTC emissions due to migration, the net effect of migration in China has been a reduction of PM2.5 exposure, primarily because of an unequal distribution of RTC energy mixes between urban and rural areas. After migration, people have switched to cleaner fuel types, which considerably lessened regional emissions. Consequently, the national average PM2.5 exposure concentration in 2010 was reduced by 3.9 μg/m3 (90% confidence interval, 3.0 to 5.4 μg/m3) due to migration, corresponding to an annual reduction of 36,000 (19,000 to 47,000) premature deaths. This reduction was the result of an increase in deaths by 142,000 (78,000 to 181,000) due to migrants swarming into cities and decreases in deaths by 148,000 (76,000 to 194,000) and 29,000 (15,000 to 39,000) due to transitions to a cleaner energy mix and lower urban population densities, respectively. Locally, however, megacities such as Beijing and Shanghai experienced increases in PM2.5 exposure associated with migration because these cities received massive immigration, which has driven a large increase in local emissions.

Spatial and Temporal Trends in Global Emissions of Nitrogen Oxides from 1960 to 2014

The quantification of nitrogen oxide (NOx) emissions is critical for air quality modeling. Based on updated fuel consumption and emission factor databases, a global emission inventory was compiled with high spatial (0.1° × 0.1°), temporal (monthly), and source (87 sources) resolutions for the period 1960 to 2014. The monthly emission data have been uploaded online ( http://inventory.pku.edu.cn ), along with a number of other air pollutant and greenhouse gas data for free download. Differences in source profiles, not global total quantities, between our results and those reported previously were found. There were significant differences in total and per capita emissions and emission intensities among countries, especially between the developing and developed countries. Globally, the total annual NOx emissions finally stopped increasing in 2013 after continuously increasing over several decades, largely due to strict control measures taken in China in recent years. Nevertheless, the peak year of NOx emissions was later than for many other major air pollutants. Per capita emissions, either among countries or over years, follow typical inverted U-shaped environmental Kuznets curves, indicating that the emissions increased during the early stage of development and were restrained when socioeconomic development reached certain points. Although the trends are similar among countries, the turning points of developing countries appeared sooner than those of developed countries in terms of development status, confirming late-move advantages.

Origin and Radiative Forcing of Black Carbon Aerosol: Production and Consumption Perspectives

Air pollution, a threat to air quality and human health, has attracted ever-increasing attention in recent years. In addition to having local influence, air pollutants can also travel the globe via atmospheric circulation and international trade. Black carbon (BC), emitted from incomplete combustion, is a unique but representative particulate pollutant. This study tracked down the BC aerosol and its direct radiative forcing to the emission sources and final consumers using the global chemical transport model (MOZART-4), the rapid radiative transfer model for general circulation simulations (RRTM), and a multiregional input-output analysis (MRIO). BC was physically transported (i.e., atmospheric transport) from western to eastern countries in the midlatitude westerlies, but its magnitude is near an order of magnitude higher if the virtual flow embodied in international trade is considered. The transboundary effects on East and South Asia by other regions increased from about 3% (physical transport only) to 10% when considering both physical and virtual transport. The influence efficiency on East Asia was also large because of the comparatively large emission intensity and emission-intensive exports (e.g., machinery and equipment). The radiative forcing in Africa imposed by consumption from Europe, North America, and East Asia (0.01 Wm-2) was even larger than the total forcing in North America. Understanding the supply chain and incorporating both atmospheric and virtual transport may improve multilateral cooperation on air pollutant mitigation both domestically and internationally.

A novel enhanced diffusion sampler for collecting gaseous pollutants without air agitation

ABSTRACT A novel enhanced diffusion sampler for collecting gaseous phase polycyclic aromatic hydrocarbons (PAHs) without air agitation is proposed. The diffusion of target compounds into a sampling chamber is facilitated by continuously purging through a closed-loop flow to create a large concentration difference between the ambient air and the air in the sampling chamber. A glass-fiber filter-based prototype was developed. It was demonstrated that the device could collect gaseous PAHs at a much higher rate (1.6 ± 1.4 L/min) than regular passive samplers, while the ambient air is not agitated. The prototype was also tested in both the laboratory and field for characterizing the concentration gradients over a short distance from the soil surface. The sampler has potential to be applied in other similar situations to characterize the concentration profiles of other chemicals.

Distinguishing Emission-Associated Ambient Air PM2.5 Concentrations and Meteorological Factor-Induced Fluctuations

Although PM2.5 (particulate matter with aerodynamic diameters less than 2.5 μm) in the air originates from emissions, its concentrations are often affected by confounding meteorological effects. Therefore, direct comparisons of PM2.5 concentrations made across two periods, which are commonly used by environmental protection administrations to measure the effectiveness of mitigation efforts, can be misleading. Here, we developed a two-step method to distinguish the significance of emissions and meteorological factors and assess the effectiveness of emission mitigation efforts. We modeled ambient PM2.5 concentrations from 1980 to 2014 based on three conditional scenarios: realistic conditions, fixed emissions, and fixed meteorology. The differences found between the model outputs were analyzed to quantify the relative contributions of emissions and meteorological factors. Emission-related gridded PM2.5 concentrations excluding the meteorological effects were predicted using multivariate regression models, whereas meteorological confounding effects on PM2.5 fluctuations were characterized by probabilistic functions. When the regression models and probabilistic functions were combined, fluctuations in the PM2.5 concentrations induced by emissions and meteorological factors were quantified for all model grid cells and regions. The method was then applied to assess the historical and future trends of PM2.5 concentrations and potential fluctuations on global, national, and city scales. The proposed method may thus be used to assess the effectiveness of mitigation actions.