Yuanchen Chen

Global atmospheric emissions of polycyclic aromatic hydrocarbons from 1960 to 2008 and future predictions.

Global atmospheric emissions of 16 polycyclic aromatic hydrocarbons (PAHs) from 69 major sources were estimated for a period from 1960 to 2030. Regression models and a technology split method were used to estimate country and time specific emission factors, resulting in a new estimate of PAH emission factor variation among different countries and over time. PAH emissions in 2007 were spatially resolved to 0.1° × 0.1° grids based on a newly developed global high-resolution fuel combustion inventory (PKU-FUEL-2007). The global total annual atmospheric emission of 16 PAHs in 2007 was 504 Gg (331-818 Gg, as interquartile range), with residential/commercial biomass burning (60.5%), open-field biomass burning (agricultural waste burning, deforestation, and wildfire, 13.6%), and petroleum consumption by on-road motor vehicles (12.8%) as the major sources. South (87 Gg), East (111 Gg), and Southeast Asia (52 Gg) were the regions with the highest PAH emission densities, contributing half of the global total PAH emissions. Among the global total PAH emissions, 6.19% of the emissions were in the form of high molecular weight carcinogenic compounds and the percentage of the carcinogenic PAHs was higher in developing countries (6.22%) than in developed countries (5.73%), due to the differences in energy structures and the disparities of technology. The potential health impact of the PAH emissions was greatest in the parts of the world with high anthropogenic PAH emissions, because of the overlap of the high emissions and high population densities. Global total PAH emissions peaked at 592 Gg in 1995 and declined gradually to 499 Gg in 2008. Total PAH emissions from developed countries peaked at 122 Gg in the early 1970s and decreased to 38 Gg in 2008. Simulation of PAH emissions from 2009 to 2030 revealed that PAH emissions in developed and developing countries would decrease by 46-71% and 48-64%, respectively, based on the six IPCC SRES scenarios.

Black carbon emissions in China from 1949 to 2050.

Black carbon (BC) emissions from China are of global concern. A new BC emission inventory (PKU-BC(China)) has been developed with the following improvements: (1) The emission factor database was updated; (2) a 0.1° × 0.1° gridded map was produced for 2007 based on county-level proxies; (3) time trends were derived for 1949-2007 and predicted for 2008-2050; and (4) the uncertainties associated with the inventory were quantified. It was estimated that 1957 Gg of BC were emitted in China in 2007, which is greater than previously reported. Residential coal combustion was the largest source, followed by residential biofuel burning, coke production, diesel vehicles, and brick kilns. By using a county-level disaggregation method, spatial bias in province-level disaggregation, mainly due to uneven per capita emissions within provinces, was reduced by 42.5%. Emissions increased steadily since 1949 until leveling off in the mid-1990s, due to a series of technological advances and to socioeconomic progress. BC emissions in China in 2050 are predicted to be 920-2183 Gg/yr under various scenarios; and the industrial and transportation sectors stand to benefit the most from technological improvements.

Emissions of Parent, Nitro, and Oxygenated Polycyclic Aromatic Hydrocarbons from Residential Wood Combustion in Rural China

Residential wood combustion is one of the important sources of air pollution in developing countries. Among the pollutants emitted, parent polycyclic aromatic hydrocarbons (pPAHs) and their derivatives, including nitrated and oxygenated PAHs (nPAHs and oPAHs), are of concern because of their mutagenic and carcinogenic effects. In order to evaluate their impacts on regional air quality and human health, emission inventories, based on realistic emission factors (EFs), are needed. In this study, the EFs of 28 pPAHs (EF(PAH28)), 9 nPAHs (EF(PAHn9)), and 4 oPAHs (EF(PAHo4)) were measured for residential combustion of 27 wood fuels in rural China. The measured EF(PAH28), EF(PAHn9), and EF(PAHo4) for brushwood were 86.7 ± 67.6, 3.22 ± 1.95 × 10(-2), and 5.56 ± 4.32 mg/kg, which were significantly higher than 12.7 ± 7.0, 8.27 ± 5.51 × 10(-3), and 1.19 ± 1.87 mg/kg for fuel wood combustion (p < 0.05). Sixteen U.S. EPA priority pPAHs contributed approximately 95% of the total of the 28 pPAHs measured. EFs of pPAHs, nPAHs, and oPAHs were positively correlated with one another. Measured EFs varied obviously depending on fuel properties and combustion conditions. The EFs of pPAHs, nPAHs, and oPAHs were significantly correlated with modified combustion efficiency and fuel moisture. Nitro-naphthalene and 9-fluorenone were the most abundant nPAHs and oPAHs identified. Both nPAHs and oPAHs showed relatively high tendencies to be present in the particulate phase than pPAHs due to their lower vapor pressures. The gas-particle partitioning of freshly emitted pPAHs, nPAHs, and oPAHs was primarily controlled by organic carbon absorption.

Field Measurement of Emission Factors of PM, EC, OC, Parent, Nitro-, and Oxy- Polycyclic Aromatic Hydrocarbons for Residential Briquette, Coal Cake, and Wood in Rural Shanxi, China

Air pollutants from residential solid fuel combustion are attracting growing public concern. Field measured emission factors (EFs) of various air pollutants for solid fuels are close to the reality and urgently needed for better emission estimations. In this study, emission factors of particulate matter (PM), organic carbon (OC), elemental carbon (EC), and various polycyclic aromatic hydrocarbons (PAHs) from residential combustions of coal briquette, coal cake, and wood were measured in rural Heshun County, China. The measured EFs of PM, OC, and EC were 8.1-8.5, 2.2-3.6, 0.91-1.6 g/kg for the wood burnt in a simple metal stove, 0.54-0.64, 0.13-0.14, 0.040-0.0041 g/kg for the briquette burned in an improved stove with a chimney, and 3.2-8.5, 0.38-0.58, 0.022-0.052 g/kg for the homemade coal cake combusted in a brick stove with a flue, respectively. EFs of 28 parent PAHs, 4 oxygenated PAHs, and 9 nitro-PAHs were 182-297, 7.8-10, 0.14-0.55 mg/kg for the wood, 14-16, 1.7-2.6, 0.64-0.83 mg/kg for the briquette, and 168-223, 4.7-9.5, 0.16-2.4 mg/kg for the coal cake, respectively. Emissions from the wood and coal cake combustions were much higher than those for the coal briquette, especially true for high molecular weight PAHs. Most EFs measured in the field were higher than those measured in stove combustions under laboratory conditions.

Exposure to ambient black carbon derived from a unique inventory and high-resolution model

Significance In this study, we have developed a unique global black carbon (BC) emission inventory using a 10-km grid based on the latest source and emission factor information. The inventory is used to model BC concentrations using a global atmospheric aerosol climate model, with a high-resolution grid for Asia, to better resolve the exposure of populations to elevated BC concentration. The model with even higher resolution (10 km) is used for the North China Plain. Finally, the population exposure concentrations are evaluated. Black carbon (BC) is increasingly recognized as a significant air pollutant with harmful effects on human health, either in its own right or as a carrier of other chemicals. The adverse impact is of particular concern in those developing regions with high emissions and a growing population density. The results of recent studies indicate that BC emissions could be underestimated by a factor of 2–3 and this is particularly true for the hot-spot Asian region. Here we present a unique inventory at 10-km resolution based on a recently published global fuel consumption data product and updated emission factor measurements. The unique inventory is coupled to an Asia-nested (∼50 km) atmospheric model and used to calculate the global population exposure to BC with fully quantified uncertainty. Evaluating the modeled surface BC concentrations against observations reveals great improvement. The bias is reduced from −88% to −35% in Asia when the unique inventory and higher-resolution model replace a previous inventory combined with a coarse-resolution model. The bias can be further reduced to −12% by downscaling to 10 km using emission as a proxy. Our estimated global population-weighted BC exposure concentration constrained by observations is 2.14 μg⋅m−3; 130% higher than that obtained using less detailed inventories and low-resolution models.

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.

Emission Characteristics for Polycyclic Aromatic Hydrocarbons from Solid Fuels Burned in Domestic Stoves in Rural China

Emission characterization of polycyclic aromatic hydrocarbons (PAHs) from residential combustion of crop residues, woody material, coal, and biomass pellets in domestic stoves in rural China are compared in term of emission factors (EFs), influencing factors, composition profiles, isomer ratios and phase distributions. The EFs of PAHs vary by 2 orders of magnitude among fuel types suggesting that a detailed fuel categorization is useful in the development of an emission inventory and potential in emission abatement of PAHs by replacing dirty fuels with relatively cleaner ones. The influence of fuel moisture in biomass burning is nonlinear. Biofuels with very low moisture display relatively high emissions as do fuels with very high moisture. Bituminous coals and brushwood yield relatively large fractions of high molecular PAHs. The emission factor of benzo(a)pyrene equivalent quantity for raw bituminous coal is as high as 52 mg/kg, which is 1-2 orders of magnitude higher than the other fuels. For source diagnosis, high molecular weight isomers are more informative than low molecular weight ones and multiple ratios could be used together whenever possible.

Trend in Global Black Carbon Emissions from 1960 to 2007

Black carbon (BC) plays an important role in both climate change and health impact. Still, BC emissions as well as the historical trends are associated with high uncertainties in existing inventories. In the present study, global BC emissions from 1960 to 2007 were estimated for 64 sources, by using recompiled fuel consumption and emission factor data sets. Annual BC emissions had increased from 5.3 (3.4-8.5 as an interquartile range) to 9.1 (5.6-14.4) teragrams during this period. Our estimations are 11-16% higher than those in previous inventories. Over the period, we found that the BC emission intensity, defined as the amount of BC emitted per unit of energy production, had decreased for all the regions, especially China and India. Improvements in combustion technology and changes in fuel composition had led to an increase in energy use efficiency, and subsequently a decline of BC emission intensities in power plants, the residential sector, and transportation. On the other hand, the BC emission intensities had increased in the industrial and agricultural sectors, mainly due to an expansion of low-efficiency industry (coke and brick production) in developing countries and to an increasing usage of diesel in agriculture in developed countries.

Global lung cancer risk from PAH exposure highly depends on emission sources and individual susceptibility

The health impacts of polycyclic aromatic hydrocarbons (PAHs), the most concerning organic pollutants, depend not only on the locations and strengths of emission sources, but also on individual susceptibility. Moreover, trans-boundary transport makes them a global concern. In this study, a comprehensive analysis of the global health impacts of polycyclic aromatic hydrocarbons (PAHs) in ambient air is presented. Model resolution is critical in exposure modelling. Globally, incremental lifetime lung cancer risk (ILCR) induced by ambient PAH exposure is 3.1 × 10−5. If the individual susceptibility was not taken into consideration, the overall risk would be underestimated by 55% and the proportion of highly vulnerable population would be underestimated by more than 90%. Emphasizing on individual susceptibility, our study provides an instrumental revision of current risk assessment methodology. In terms of lung cancer risk, the most important sources are combustion of biomass fuels (40%) and fossil fuels (14%) in the residential/commercial sector, coke (13%) and aluminium (12%) production, and motor vehicles (9%). PAHs can travel long distance globally especially within the Eurasian continent. Still, the risk is dominantly contributed by local.

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.