Using Machine Learning to Construct the Blood-Follicle Distribution Models of Various Trace Elements and Explore the Transport-Related Pathways with Multiomics Data.

Permeabilities of various trace elements (TEs) through the blood-follicle barrier (BFB) play an important role in oocyte development. However, it has not been comprehensively described as well as its involved biological pathways. Our study aimed to construct a blood-follicle distribution model of the concerned TEs and explore their related biological pathways. We finally included a total of 168 women from a cohort of in vitro fertilization-embryo transfer conducted in two reproductive centers in Beijing City and Shandong Province, China. The concentrations of 35 TEs in both serum and follicular fluid (FF) samples from the 168 women were measured, as well as the multiomics features of the metabolome, lipidome, and proteome in both plasma and FF samples. Multiomics features associated with the transfer efficiencies of TEs through the BFB were selected by using an elastic net model and further utilized for pathway analysis. Various machine learning (ML) models were built to predict the concentrations of TEs in FF. Overall, there are 21 TEs that exhibited three types of consistent BFB distribution characteristics between Beijing and Shandong centers. Among them, the concentrations of arsenic, manganese, nickel, tin, and bismuth in FF were higher than those in the serum with transfer efficiencies of 1.19-4.38, while a reverse trend was observed for the 15 TEs with transfer efficiencies of 0.076-0.905, e.g., mercury, germanium, selenium, antimony, and titanium. Lastly, cadmium was evenly distributed in the two compartments with transfer efficiencies of 0.998-1.056. Multiomics analysis showed that the enrichment of TEs was associated with the synthesis and action of steroid hormones and the glucose metabolism. Random forest model can provide the most accurate predictions of the concentrations of TEs in FF among the concerned ML models. In conclusion, the selective permeability through the BFB for various TEs may be significantly regulated by the steroid hormones and the glucose metabolism. Also, the concentrations of some TEs in FF can be well predicted by their serum levels with a random forest model.

Identification of Factors Determining Household PM2.5 Variations at Regional Scale and Their Implications for Pollution Mitigation.

Indoor PM2.5, particulate matter no more than 2.5 µm in aerodynamic equivalent diameter, has very high spatiotemporal variabilities; and exploring the key factors influencing the variabilities is critical for purifying air and protecting human health. Here, we conducted a longer-term field monitoring campaign using low-cost sensors and evaluated inter- and intra-household PM2.5 variations in rural areas where energy or stove stacking is common. Household PM2.5 varied largely across different homes but also within households. Using generalized linear models and dominance analysis, we estimated that outdoor PM2.5 explained 19% of the intrahousehold variation in indoor daily PM2.5, whereas factors like the outdoor temperature and indoor-outdoor temperature difference that was associated with energy use directly or indirectly, explained 26% of the temporal variation. Inter-household variation was lower than intrahousehold variation. The inter-household variation was strongly associated with distinct internal sources, with energy-use-associated factors explaining 35% of the variation. The statistical source apportionment model estimated that solid fuel burning for heating contributed an average of 31%-55% of PM2.5 annually, whereas the contribution of sources originating from the outdoors was ≤10%. By replacing raw biomass or coal with biomass pellets in gasifier burners for heating, indoor PM2.5 could be significantly reduced and indoor temperature substantially increased, providing thermal comforts in addition to improved air quality.

PAHs bound to submicron particles in rural Chinese homes burning solid fuels.

Inhalation exposure to polycyclic aromatic hydrocarbons (PAHs) from indoor solid fuel combustion poses a high health risk, and PAHs bound to particles with smaller sizes (e.g., PM1.0, aerodynamic diameter ≤ 1.0 µm) should be of particular concern since they can penetrate deep into pulmonary alveoli. However, PAHs bound to PM1.0 was less studied compared with PAHs in total suspended particles or PM2.5. In this study, multiple provincial field measurements were conducted to investigate 28 PAHs bound to PM1.0 in rural Chinese homes. Daily averaged PM1.0-PAH28 concentrations ranged from 27 ng/m3 to 3795 ng/m3 (median: 233 ng/m3) and from 10 ng/m3 to 2978 ng/m3 (median: 87 ng/m3) in indoor and outdoor air, respectively. Higher concentrations were found in northern China in winter due to increased solid fuels consumption for space heating. The ambient pollution was lower during the non-heating season in Eastern China, where clean energy was preferred. Highly toxic congeners were more abundant in indoor air compared with outdoor air. The results of source apportionment revealed that solid fuel combustion was the primary contributor to rural household PM1.0-PAHs, but other sources such as vehicles cannot be overlooked. The transition to cleaner energy can reduce the indoor PM1.0-PAH28 and BaPeq-28 concentrations by 87% and 98%, respectively, and more efficient reduction was observed for highly toxic congeners. The estimated Incremental Lifetime Cancer Risk (ILCR) based on PM1.0-PAH28 ranged from 4.6 × 10-5 to 3.4 × 10-2, far exceeding the acceptable level of 10-6. Over 60% of the ILCR could be attributed to inhalation exposure during childhood and adolescence.

Mass Absorption Efficiency of Black Carbon from Residential Solid Fuel Combustion and Its Association with Carbonaceous Fractions.

Black carbon (BC) emissions, derived primarily from incomplete fuel combustion, significantly affect the global and regional climate. Mass absorption efficiency (MAE) is one important parameter in evaluating the climate impacts of BC. Here, values and variabilities in the MAE of BC (MAEBC) from real-world residential emissions were investigated from a field campaign covering 163 burning events for different fuel-stove combinations. MAEBC (average: 12 ± 5 m2/g) was normally distributed and varied greatly by 2 orders of magnitude. Statistically significant differences in MAEBC were found for various fuels, while no significant differences were observed among different stoves. The fuel difference explained 72 ± 7% of the MAEBC variation. MAEBC did not correlate with the modified combustion efficiency but positively correlated with the ratio of organic carbon (OC) to elemental carbon (EC) and negatively correlated with char-EC. The OC/EC ratio was not always lower in coal emissions in comparison to biomass burning emissions. Coal- and biomass-burning emissions had different profiles of carbon fractions. Char-EC, OC, OC/EC, and char-EC/soot-EC can explain 68.7% of the MAEBC variation, providing the potential for predicting MAEBC from the carbon fractions, since they are more commonly measured and available.

Optically Measured Black and Particulate Brown Carbon Emission Factors from Real-World Residential Combustion Predominantly Affected by Fuel Differences.

Residential solid fuel use is an important source of black carbon (BC) but also a main source of uncertainty in BC emission inventories, as reliable real-world emission factors (EFs) and data on consumption of noncommercial household fuels are limited. In this study, particulate BC and brown carbon (BrC) for real-world indoor coal and biomass burning were evaluated using a SootScan model OT21 optical transmissometer from a field campaign including 343 biomass/coal combustion events. The highest BC EF from the burning of coal cake (a mixed fuel locally made from coal and clay) was 1.6-6.4 higher than that of other fuels, and BC EFs were higher for coal combustion than for biomass burning. The highest particulate BrC EF was from charcoal burning and was 1.5-4.3 times higher than that from other biomass and coals. Burning fuel in iron stoves had lower BC and BrC EFs, at approximately 15-66% and 40-54%, respectively, compared with burning in other stove types. The difference between heating and cooking activities was statistically insignificant (p > 0.05). A generalized linear model coupled with dominance analysis evidenced that the EFs were significantly associated with fuel and stove types, with the fuel difference being a major influencing factor explaining 68% of the variation. This suggests that a clean fuel transition would have beneficial impacts on air pollution associated with the residential sector in China. The absorption EFs differed by 2-3 orders of magnitude across different fuel-stove combinations. The Absorption Ångström Exponent values for the particulate from residential solid fuel combustions ranged from 0.92 to 3.7.

Spatially Resolved Emission Factors to Reduce Uncertainties in Air Pollutant Emission Estimates from the Residential Sector.

The residential sector is a major source of air pollutant emission inventory uncertainties. A nationwide field emission measurement campaign was conducted in rural China to evaluate the variabilities of realistic emission factors (EFs) from indoor solid fuel combustion. For a total of 1313 burning events, the overall average EFs (±standard deviation) of PM2.5 were 8.93 ± 6.95 and 7.33 ± 9.01 g/kg for biomass and coals, respectively, and 89.3 ± 51.2 and 114 ± 87 g/kg for CO. Higher EFs were found from burning of uncompressed straws, while lower EFs were found from processed biomass pellets, coal briquettes, and relatively clean anthracite coals. Modified combustion efficiency was found to be the most significant factor associated with variations in CO EFs, whereas for PM2.5, fuel and stove differences determined its variations. Weak correlations between PM2.5 and CO indicated high uncertainties in using CO as a surrogate for PM2.5. EFs accurately fit log-normal distributions, and obvious spatial heterogeneity was observed attributed to different fuel-stove combinations across the country. Emission estimation variabilities, which are determined by the interquartile ranges divided by the median values, were notably reduced when spatially resolved EFs were adopted in the inventory.

Organochlorine Pesticide Ban Facilitated Reproductive Recovery of Chinese Striped Hamsters.

Organochlorine pesticides (OCPs) have been used worldwide on an enormous scale over the last century but are banned globally due to environmental persistence and ecotoxicity in recent decades. The long-term effects of OCP ban for agricultural use in China since 1983 on the reproductive health of small terrestrial mammals have never been evaluated in the field. We examined the residue dynamics of OCPs and the reproductive performance of Chinese striped hamsters (Cricetulus barabensis) in North China Plain during 1983-2010 and concluded that the exposure levels of OCPs in hamsters drastically decreased from 2900 ± 740 to 25.2 ± 6.88 ng/g with an average half-life of 5.08 yrs, coinciding with the observed reproductive recovery of hamsters. The population-based reproductive performance of hamsters was significantly and negatively associated with OCP exposure levels after adjusting the contributions from climate and population density factors, indicating that the ban of OCPs has facilitated the reproductive recovery of hamsters by up to 81% contribution. Our findings suggest that the OCP ban is effective to restore reproduction of small terrestrial mammals. Integration of population biology and environmental science is essential to assess the impacts of persistent organic pollutants on ecological safety and biodiversity loss under accelerated global change.

Impacts of Chinese spring festival on household PM2.5 pollution and blood pressure of rural residents.

BACKGROUND: Household air pollution (HAP) from residential combustion considerably affects human health in rural China. Large-scale population migration and rural lifestyle changes during the Spring Festival are supposed to change the household air pollution and health risks; however, limited field study has determined its impacts on HAP and short-term health outcomes. METHODS: A field study was conducted in rural areas of Southern China before and during the Spring Festival to explore the associations between HAP and blood pressure considering different factors such as cooking fuel, heating fuel, and smoking. Stationary real-time PM2.5 monitors were used to measure PM2.5 concentrations of the kitchen, living room, and yard of 156 randomly selected households. Personal exposure to PM2.5 was calculated based on the results of stationary samplers and corresponding time local residents spent in different microenvironments, and one adult resident was recruited of each family for the blood pressure measurement. RESULTS: Both personal exposure to PM2.5 and blood pressures of local residents increased during Spring Festival compared to the days before the holiday. Based on generalized linear model coupled with dominance analysis approach, it was found that personal PM2.5 exposure was positively associated with the factors of population size and the types of cooking and heating fuels with the relative contributions of approximately 82%, and systolic blood pressure (SBP, 100-120 mmHg as normal range for adults) was positively and significantly associated with personal PM2.5 exposures with the relative contribution of 11%. CONCLUSION: The findings in this study demonstrated that Spring Festival can give rise to increase of HAP and hypertension risks, also related to tremendous solid fuel use, suggesting further policy making on promoting cleaner energy in rural areas and more attention on large population migration during national holidays.

Old pesticide, new use: Smart and safe enantiomer of isocarbophos in locust control.

Locust plagues are still worldwide problems. Selecting active enantiomers from current chiral insecticides is necessary for controlling locusts and mitigating the pesticide pollution in agricultural lands. Herein, two enantiomers of isocarbophos (ICP) were separated and the enantioselectivity in insecticidal activity against the pest Locusta migratoria manilensis (L. migratoria) and mechanisms were investigated. The significant difference of LD50 between (+)-ICP (0.609 mg/kg bw) and (-)-ICP (79.412 mg/kg bw) demonstrated that (+)-ICP was a more effective enantiomer. The enantioselectivity in insecticidal activity of ICP enantiomers could be attributed to the selective affinity to acetylcholinesterase (AChE). Results of in vivo and in vitro assays suggested that AChE was more sensitive to (+)-ICP. In addition, molecular docking showed that the -CDOKER energies of (+)-ICP and (-)-ICP were 25.6652 and 24.4169, respectively, which suggested a stronger affinity between (+)-ICP and AChE. Significant selectivity also occurred in detoxifying enzymes activities (carboxylesterases (CarEs) and glutathione S-transferases (GSTs)) and related gene expressions. Suppression of detoxifying enzymes activities with (+)-ICP treatment suggested that (-)-ICP may induce the detoxifying enzyme-mediated ICP resistance. A more comprehensive understanding of the enantioselectivity of ICP is necessary for improving regulation and risk assessment of ICP.

Inhalation exposure to size-segregated fine particles and particulate PAHs for the population burning biomass fuels in the Eastern Tibetan Plateau area.

Indoor biomass burning produces large amounts of small particles and hazardous contaminants leading to severe air pollution and potentially high health risks associated with inhalation exposure. Personal samplers provide more accurate estimates of inhalation exposure. In this study, inhalation exposure to size-segregated particles and particulate polycyclic aromatic hydrocarbons (PAHs) for the biomass user was studied by deploying personal samplers. The study found that daily PM2.5 inhalation exposure level was as high as 121 ± 96 µg/m3, and over 84% was finer PM1.0. For PAHs, the exposure level was 113 ± 188 ng/m3, with over 77% in PM1.0. High molecular weight PAHs with larger toxic potentials enriched in smaller particles resulting in much high risks associated with PAHs inhalation exposure. Indoor exposure contributed to ~80% of the total inhalation exposure as a result of high indoor air pollution and longer residence spent indoor. The highest exposure risk was found for the male smoker who conducted cooking activities at home.

Rapid Increase in Cement-Related Mercury Emissions and Deposition in China during 2005-2015.

The cement industry has become the largest mercury (Hg) emission source in China. Better understanding Hg emission and deposition characteristics and drivers of Hg emission changes can increase the awareness of related risks and support effective policy making. The results show that due to the substantial increase in the use of new suspension preheater and precalciner (NSP) technology in China, an approximate two-fold increase from 80.0 to 144.0 Mg year-1 was observed for the cement-related Hg emissions during 2005-2015, which has resulted in a considerable increase in atmospheric deposition over terrestrial China from 37.9 to 75.9 Mg year-1. Compared to the great majority of emission sectors, the same increase in Hg emissions from cement production can cause more deposition due to the large share of highly water-soluble divalent Hg in the sector. Each 1% increase in the share of divalent Hg can result in an increase of 0.37 Mg year-1 in deposition over terrestrial China. Technical improvement and diversification of cement products are two major driving forces offsetting the economy-induced growth in cement-related Hg emissions during 2005-2015. Measures aimed at reducing the Hg emission intensity against the further increase in the use of NSP technology and avoiding overcapacity against the stimulation of real estate and increasing cement demands are urgently needed for the cement industry in China.

Resolution of the Ongoing Challenge of Estimating Nonpoint Source Neonicotinoid Pollution in the Yangtze River Basin Using a Modified Mass Balance Approach.

Neonicotinoid insecticides have been widely consumed worldwide, particularly in China. There is a growing interest in the environmental research community about the occurrence, fates, sources, and risks of neonicotinoids. Nine neonicotinoids in river/lake water were measured at 12 sites along the Yangtze River Basin during the dry and wet seasons in 2016, and nonpoint sources were also identified based on a modified mass balance method. A significantly higher concentration of neonicotinoids was found during the dry season probably due to the dilution effect and insecticide consumption. The high pollution levels are due to posing high ecological risks compared with the recommended thresholds. In 2016, 1190 (95% confidence interval (CI) = 822-1690) tons of neonicotinoids were transferred into the adjacent sea. Nonpoint source pollution (1700 (CI = 1200-2370) tons) was the major contributor (91.3%) to the total input of neonicotinoids into the system. Composition profiles identifying specific neonicotinoid sources indicated some changes in usage patterns from old to new types of neonicotinoids. This spatial and seasonal field study and source identification is expected to fill the data gap regarding the limited information on neonicotinoid use patterns and to inform further effective policy-making and intervention programs in China that should be urgently promoted in the near future.

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

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.

Air pollution and inhalation exposure to particulate matter of different sizes in rural households using improved stoves in central China.

Household air pollution is considered to be among the top environmental risks in China. To examine the performance of improved stoves for reduction of indoor particulate matter (PM) emission and exposure in rural households, individual inhalation exposure to size-resolved PM was investigated using personal portable samplers carried by residents using wood gasifier stoves or improved coal stoves in a rural county in Central China. Concentrations of PM with different sizes in stationary indoor and outdoor air were also monitored at paired sites. The stationary concentrations of size-resolved PM in indoor air were greater than those in outdoor air, especially finer particles PM0.25. The daily averaged exposure concentrations of PM0.25, PM1.0, PM2.5 and total suspended particle for all the surveyed residents were 74.4±41.1, 159.3±74.3, 176.7±78.1 and 217.9±78.1µg/m3, respectively. Even using the improved stoves, the individual exposure to indoor PM far exceeded the air quality guideline by WHO at 25µg/m3. Submicron particles PM1.0 were the dominant PM fraction for personal exposure and indoor and outdoor air. Personal exposure exhibited a closer correlation with indoor PM concentrations than that for outdoor concentrations. Both inhalation exposure and indoor air PM concentrations in the rural households with gasifier firewood stoves were evidently lower than the reported results using traditional firewood stoves. However, local governments in the studied rural areas should exercise caution when widely and hastily promoting gasifier firewood stoves in place of improved coal stoves, due to the higher PM levels in indoor and outdoor air and personal inhaled exposure.

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

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.

Polycyclic aromatic hydrocarbons in ambient air, surface soil and wheat grain near a large steel-smelting manufacturer in northern China.

The total concentrations and component profiles of polycyclic aromatic hydrocarbons (PAHs) in ambient air, surface soil and wheat grain collected from wheat fields near a large steel-smelting manufacturer in Northern China were determined. Based on the specific isomeric ratios of paired species in ambient air, principle component analysis and multivariate linear regression, the main emission source of local PAHs was identified as a mixture of industrial and domestic coal combustion, biomass burning and traffic exhaust. The total organic carbon (TOC) fraction was considerably correlated with the total and individual PAH concentrations in surface soil. The total concentrations of PAHs in wheat grain were relatively low, with dominant low molecular weight constituents, and the compositional profile was more similar to that in ambient air than in topsoil. Combined with more significant results from partial correlation and linear regression models, the contribution from air PAHs to grain PAHs may be greater than that from soil PAHs.

Pollutant emissions from improved coal- and wood-fuelled cookstoves in rural households.

Residential solid fuel combustion is a major source of many pollutants, resulting in significant impacts on air quality and human health. Improved stoves, especially some modern gasifier biomass models, are being deployed to alleviate household and ambient air pollution. Pollutant emissions from coal burning in improved metal stoves (n = 11) and wood combustion in modern gasifier stoves (n = 8) were measured in field in Hubei, China. The emissions of CO, TSP, OC, EC, and PAHs from coal burning in the improved iron stoves were generally lower than previously reported results for coal in traditional stoves. For pollutants from wood combustion in the gasifier stoves, the emissions were less than literature-reported values for wood burned in traditional stoves, comparable to those in improved stoves, but appeared to be higher than those for pellets in gasifier stoves in laboratory tests. The limitations of scarce data and large variances result in statistical insignificance. Daily emissions of targeted pollutants per household were found to be higher for wood burners, compared with households relying on coal. The gasifier stove had relatively high thermal efficiencies, but emissions of most air pollutants per delivered energy were not significantly different from those from the coal burning in improved iron stoves. Moreover, higher emissions of OC, EC, and PAHs were observed, indicating that caution and additional testing will be needed while designing future clean cookstove intervention programs.

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.

Global mercury emissions from combustion in light of international fuel trading.

The spatially resolved emission inventory is essential for understanding the fate of mercury. Previous global mercury emission inventories for fuel combustion sources overlooked the influence of fuel trading on local emission estimates of many countries, mostly developing countries, for which national emission data are not available. This study demonstrates that in many countries, the mercury content of coal and petroleum locally consumed differ significantly from those locally produced. If the mercury content in locally produced fuels were used to estimate emission, then the resulting global mercury emissions from coal and petroleum would be overestimated by 4.7 and 72%, respectively. Even higher misestimations would exist in individual countries, leading to strong spatial bias. On the basis of the available data on fuel trading and an updated global fuel consumption database, a new mercury emission inventory for 64 combustion sources has been developed. The emissions were mapped at 0.1° × 0.1° resolution for 2007 and at country resolution for a period from 1960 to 2006. The estimated global total mercury emission from all combustion sources (fossil fuel, biomass fuel, solid waste, and wildfires) in 2007 was 1454 Mg (1232-1691 Mg as interquartile range from Monte Carlo simulation), among which elementary mercury (Hg(0)), divalent gaseous mercury (Hg(2+)), and particulate mercury (Hg(p)) were 725, 548, and 181 Mg, respectively. The total emission from anthropogenic sources, excluding wildfires, was 1040 Mg (886-1248 Mg), with coal combustion contributing more than half. Globally, total annual anthropogenic mercury emission from combustion sources increased from 285 Mg (263-358 Mg) in 1960 to 1040 Mg (886-1248 Mg) in 2007, owing to an increased fuel consumption in developing countries. However, mercury emissions from developed countries have decreased since 2000.

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.