Xi Zhu

Household air pollution and personal exposure to nitrated and oxygenated polycyclic aromatics (PAHs) in rural households: Influence of household cooking energies.

Residential solid fuels are widely consumed in rural China, contributing to severe household air pollution for many products of incomplete combustion, such as polycyclic aromatic hydrocarbons (PAHs) and their polar derivatives. In this study, concentrations of nitrated and oxygenated PAH derivatives (nPAHs and oPAHs) for household and personal air were measured and analyzed for influencing factors like smoking and cooking energy type. Concentrations of nPAHs and oPAHs in kitchens were higher than those in living rooms and in outdoor air. Exposure levels measured by personal samplers were lower than levels in indoor air, but higher than outdoor air levels. With increasing molecular weight, individual compounds tended to be more commonly partitioned to particulate matter (PM); moreover, higher molecular weight nPAHs and oPAHs were preferentially found in finer particles, suggesting a potential for increased health risks. Smoking behavior raised the concentrations of nPAHs and oPAHs in personal air significantly. People who cooked food also had higher personal exposures. Cooking and smoking have a significant interaction effect on personal exposure. Concentrations in kitchens and personal exposure to nPAHs and oPAHs for households using wood and peat were significantly higher than for those using electricity and liquid petroleum gas (LPG).

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.

Properties and cellular effects of particulate matter from direct emissions and ambient sources

ABSTRACT The pollution of particulate matter (PM) is of great concern in China and many other developing countries. It is generally recognized that the toxicity of PM is source and property dependent. However, the relationship between PM properties and toxicity is still not well understood. In this study, PM samples from direct emissions of wood, straw, coal, diesel combustion, cigarette smoking and ambient air were collected and characterized for their physicochemical properties. Their expression of intracellular reactive oxygen species (ROS) and levels of inflammatory cytokines (i.e., tumor necrosis factor-α (TNF-α)) was measured using a RAW264.7 cell model. Our results demonstrated that the properties of the samples from different origins exhibited remarkable differences. Significant increases in ROS were observed when the cells were exposed to PMs from biomass origins, including wood, straw and cigarettes, while increases in TNF-α were found for all the samples, particularly those from ambient air. The most important factor associated with ROS generation was the presence of water-soluble organic carbon, which was extremely abundant in the samples that directly resulted from biomass combustion. Metals, endotoxins and PM size were the most important properties associated with increases in TNF-α expression levels. The association of the origins of PM particles and physicochemical properties with cytotoxic properties is illustrated using a cluster analysis.

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.

Field-based emission measurements of biomass burning in typical Chinese built-in-place stoves

Residential combustion emission contributes significantly to ambient and indoor air pollution in China; however, this pollution source is poorly characterized and often overlooked in national pollution control policies. Few studies, and even fewer field-based investigations, have evaluated pollutant emissions from indoor biomass burning. One significant feature of Chinese household biofuel stoves is that many are built on site. In this study, 112 tests were conducted to investigate pollutant emission factors and variations for 11 fuel-stove combinations in actual use in the field. Results showed that, compared to those emission tests under controlled fuel burning conditions, EFs of methane, sulfur dioxide, particulate matter, and organic carbon from the field-based uncontrolled tests were higher, but carbon monoxide, nitrogen oxides, and elemental carbon were not significantly different. Controlled burning tests may be unrepresentative of real-world fuel burning. Pollutant emissions from uncontrolled burning tests had much higher variations compared with controlled tests. Most pollutant emissions from indoor straw burning are higher than that in open burning, except nitrogen oxides. The typical built-in-place home stoves in China had low efficiencies and high pollutant emissions that were rated as Tier 0 (the worst) or Tier 1 of a four-tier scale according to the International Organization for Standardization, International Workshop Agreement 11-2012. Effective interventions are expected to lower pollutant emissions from residential combustion to improve air quality and to protect human health.

Fluctuation in time-resolved PM2.5 from rural households with solid fuel-associated internal emission sources

Indoor air contributes significantly to overall exposure, particularly for rural Chinese who often use solid fuels for cooking and/or heating. Unfortunately, overlooked rural indoor air leads to a critical knowledge gap. Simultaneous measurements in the kitchen, living room, and immediately outside of houses using six-channel particle counters were carried out in 18 biomass-burning rural and 3 non-biomass-burning urban households (as a comparison) in winter to characterize dynamic change patterns indoor air pollution and indoor-outdoor relationship. The rural households mainly used wood or crop residues for cooking and heating, while the urban households used pipelined natural gas for cooking and air conditioners for heating. In rural households with significant solid-fuel burning internal sources, the highest concentration was found in the kitchen (101 ± 56 μg/m3), with comparable levels in the living room (99 ± 46 μg/m3) and low levels in outdoor air (91 ± 39 μg/m3). A generally opposite direction of indoor-outdoor exchange was found between the rural and urban households. PM in kitchen air is smaller than that in living rooms and outdoors because solid fuel burning (mainly in rural households) and cooking oil heating (in rural and urban households). Indoor and outdoor PM concentration changed synchronously, with a slight delay in indoor air in urban households but a slight delay in outdoor air in rural households. Cooking, heating, and smoking elevated indoor PM significantly, but different from the cooking activity that produced peaks lasting for about 30 min, emissions from heating created a series of peaks due to frequent disturbance and fuel-feeding and had more significant impacts on the daily average concentration. Distinct indoor-outdoor relationships and dynamic change patterns between the two household categories w/o strong internal biomass burning sources imply that totally different model schemes are needed to quantitatively address indoor air pollution and inhalation exposure.

Seasonal and spatial variations in the chemical components and the cellular effects of particulate matter collected in Northern China

The health effects of airborne particulate matter (PM) are likely to be strongly influenced by its components. The relationship between the composition of PM and its biological effects has been investigated in vitro/vivo, but more studies are needed to achieve a better understanding of the relationship. Such studies are limited in Northern China, where severe air pollution causes significant health impacts. In this study, we analyzed seasonal PM10 (PM, aerodynamic diameter less than 10μm) samples from five typical cities in Northern China for their physicochemical properties and their in vitro effects on A549 (human lung epithelial cell line) and RAW264.7 (murine monocyte macrophage) cells, including cytotoxicity, oxidative stress and inflammatory effects. Principal component analysis and multiple linear regressions were used to investigate the relationship between the PM components and the cellular responses. The cellular responses of A549 cells were more closely related to the endotoxin content and the levels of polycyclic aromatic hydrocarbons (PAHs) and their derivatives, while the cellular responses of RAW264.7 cells were largely related to PM10-bound metals, and the chalcophile elements (Pb, Cu, Zn, Cd) were more related to the PM-induced oxidative stress, whereas the lithophile and siderophile elements (Al, Fe, Mg, Co, V, Mn, Ca) were more related to PM-induced inflammation and cytotoxicity. As PM compositions changed seasonally, more intense cellular responses were seen when A549 cells were exposed to winter samples that contained higher levels of those components. The autumn and winter samples induced higher levels of oxidative stress in RAW264.7 cells, possibly due to higher contents of chalcophile elements, whereas the spring and/or summer samples were more cytotoxic and proinflammatory, possibly due to higher contents of lithophile and siderophile elements. The study suggests that the evaluation of health impacts induced by air pollution should take into account different physiochemical properties other than the mass concentration, and that public health would benefit greatly from effective, prioritized control of the sources that are the major producers of the central species.

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.