Release of phthalate esters from a local landfill in the Tibetan Plateau: Importance of soil particle-size specific association.

High loads of phthalate esters (PAEs) in background regions can be directly attributed to the local sources, and their association with soil particles may determine the environment behaviors. However, little is known about the particle-size specific distributions of PAEs in soils from point source to the surroundings. In this study, 12 PAE congeners were measured in clay (< 2 µm), silt (2-63 µm) and sand fractions (63-250 µm) from surficial soils and soil profiles (0-200 cm) around the Lhasa landfill. The total concentrations of PAEs in bulk soils varied from 0.44 to 22.3 µg/g, with a dominance of bis(2-ethylhexyl) phthalate (DEHP). The clay-sorbed PAEs exhibited a decreasing trend with the increasing distance from landfill. This distribution pattern was well described by the Gaussian air pollution model, suggesting the airborne particles/gaseous transport of clay-sorbed PAEs. The Boltzmann equation explained the spatial variation of silt-sorbed PAEs, reflecting the atmospheric dispersion of silt-sorbed PAEs. In comparison, the sand-sorbed PAEs in surrounding soils showed downslope accumulation possibly due to the aeolian transport of sand particles. Half-life of the most abundant PAE congener DEHP was assumed based on the soil inventories from observed concentration and the Level III fugacity model simulations, and the results indicated significant longer half-life of DEHP in deeper soils (~24,000 h) than in surficial soils (5500 h). This study elucidates that the distribution and fate of soil PAEs would depend on their association with particles in the source area, and the relative stability of DEHP in deeper soils would further increase PAE inventory in soil compartment.

Polycyclic aromatic hydrocarbons in sedimentary cores of Tibetan Plateau: Influence of global warming on cold trapping.

Cold condensation is an important pathway for polycyclic aromatic hydrocarbons (PAHs) depositing at remote alpine lakes after long-range atmospheric transportation. However, in the context of global warming, the obvious temperature rise in the Tibetan Plateau (TP) might have an impact on the air deposition of PAHs by controlling the extent of cold condensation. To investigate the influence of rising temperatures on the atmospheric deposition of PAHs, two dated sedimentary cores from Pumoyum Co Lake (PC) and Selin Co Lake (SC) were collected, respectively and concentrations of 16 individual PAHs were measured. In both PC and SC, the total concentration of 16 PAHs presented relatively lower levels in four historical periods of "hot anomaly" including 1973-1975, 1988-1989, 1998-1999, and 2006-2007. This indicated that the hot temperatures might restrict the atmospheric deposition of PAHs. Besides, the results of the principal component analysis did discriminate those "hot anomalies". As the temperature kept increasing in TP, for low molecular weight PAHs and high molecular weight PAHs, the influence of rising temperatures on the cold condensation was different. Therefore, it was identified that the effect of global warming on the environmental fate of POPs cannot be neglected, especially in alpine regions like TP.

Unraveling the behaviors and significances of waste biomass ashes as underlying emission sources of soil polycyclic aromatic hydrocarbons in Tibetan Plateau.

Domestic consumption of biomass fuels has been found as a leading source of polycyclic aromatic hydrocarbons (PAHs) in pristine regions. The biomass ashes would serve as both source and vector for PAHs, which may threaten residents' health. However, research focusing on the behaviors of waste biomass ashes acting as emission resources of PAHs is still lacking. In present study, occurrence and fate of PAHs released from disposal biomass ashes in the Tibetan Plateau were investigated by evaluating their patterns and levels in soils at different distances from the Lhasa landfill. Concentrations of 16 PAHs averaged at 1009 ng/g dry weight and 103 ng/g dry weight in landfill cover soils and surrounding soils, respectively. The spatial distributions of PAHs evidenced the local source of biomass ashes in landfill, while the fractionations of PAHs in soils profiles emphasized the post-deposal leaching. Since PAH compositions altered significantly during their transport and sequestration, the rectification factors were suggested to adjust the source diagnostic ratios. In study area, the emission flux of PAHs from waste biomass ashes to soils was 0.93 ton/year; extended to the Tibetan Plateau, the flux was estimated to be 13.1-32.5 ton/year. This study confirmed that waste biomass ashes would represent significant contributions of PAH emissions in this pristine region, which might remarkably exacerbate the total emissions of PAHs in Tibet by more than 25%.

The sedimentary record of polycyclic aromatic hydrocarbons in Yamzho Yumco Lake: evolution of local sources and adsorption dynamic in the Tibetan Plateau.

With the rapid increase in anthropogenic activities, the local emissions of polycyclic aromatic hydrocarbons (PAHs) in background regions, such as the Tibetan Plateau (TP), have attracted great attention. The deposition of PAHs in lake sediments provides a historical evolutionary record of such compounds in these regions. To investigate the evolution of PAHs in the TP, two sedimentary cores from Yamzho Yumco Lake were collected and dated at high resolution, and the concentrations of 16 PAHs and sediment properties were also analyzed. The total concentrations of the 16 PAHs ranged from 6.52 to 57.97 ng/g (dry weight) in YC1 and from 0.91 to 4.57 ng/g (dry weight) in YC2. According to the methods of principal component analysis (PCA) followed by multilinear regression analysis (MLRA), four sources of PAHs in the sediments were qualitatively and quantitatively identified, such as petroleum combustion, petrogenic, coal combustion, and biomass burning. Thus, the historical evolution of PAHs was summarized. In addition, the transported distance from local PAH emission sources was found to greatly affect the composition and concentration of PAHs in sites YC1 and YC2. Specifically, local sources contributed a greater proportion of heavy molecular weight (HMW) PAHs in YC1 and a higher proportion of light-molecular-weight (LMW) PAHs in YC2. Moreover, fine particles (size < 20 µm) were found to play a significant role in adsorbing PAHs in sediments. Furthermore, ∑16PAHs in sediments were linearly correlated with the percentage of fine particles (size < 20 µm). This study provides a first example to investigate the historical evolution of PAH local emission in background regions by using lake sedimentary records, especially in the TP. Specifically, different local sources were identified using the methods of PCA followed by MLRA, and PAHs in TP sediments were predominantly adsorbed by fine particles rather than by total organic carbon (TOC) because the amount of TOC was limited.