Dissolved polycyclic aromatic hydrocarbons (PAHs-d) in response to hydrology variation and anthropogenic activities in the Yangtze River, China.

Owing to their bioavailability and toxicity, the dissolved polycyclic aromatic hydrocarbons (PAHs-d) loaded in rivers are harmful to both inland and marine ecosystems. Thus, exploring the changes in PAHs-d levels and sources is important for controlling PAHs pollution. In this study, the concentration of PAHs-d in the mainstream of the Yangtze River during dry and wet seasons was investigated and the source was analyzed using the positive matrix factorization (PMF) model to assess the response of PAHs-d to hydrological and anthropogenic activities changes. The concentration of PAHs-d in the wet season (166.2 ± 52.51 ng/L) was significantly higher than that in the dry season (89.05 ± 20.89 ng/L) (ANOVA, P < 0.001), and the sampling sites with high pollution were mainly distributed in the downstream urban agglomeration. Herein, 2-3 rings were identified to play a dominant role in the composition of PAHs-d. Compared with the dry season, the proportion of the low molecular weight (LMW) PAHs-d were relatively depleted and the high molecular weight (HMW) PAHs-d were accumulated in the wet season. Coal and coke combustion were identified as the main sources of PAHs-d (65.9% in the dry season and 59.2% in the wet season), followed by vehicle emissions, petroleum sources, and biomass combustion. Owing to the change in energy consumption structure and climate characteristics, the sources of PAHs-d displayed seasonal variation and spatial heterogeneity. Further, flow was identified as the most important factor affecting PAHs-d in the hydrological parameters. Increases of flow, pH, and SPM decreased the proportion of LMW PAHs-d, and increased that of HMW PAHs-d. The increase in anthropogenic activities intensified the residual levels of 2-3rings and 5-6 rings in water, but had no significant impact on the levels of 4 rings.

Nonhomologous Black Carbon Decoupled Char and Soot Sequestration Based on Stable Carbon Isotopes in Tibetan Plateau Lake Sediment.

Combustion-derived black carbon (BC) is an important component of sedimentary carbon pool. Due to different physicochemical properties, determining the source of char and soot is crucial for BC cycling, especially for nonhomologous char and soot in the Tibetan Plateau (TP). This study analyzed the sequestration and source of BC, char, and soot in the Dagze Co (inner TP) sediment core via the content and δ13C, revealing the biomass and fossil fuel driving on nonsynchronous char and soot and their response to local anthropogenic activities and atmospheric transmission. The results showed that BC concentration increased from 1.19 ± 0.35 mg g-1 (pre-1956) to 2.03 ± 1.05 mg g-1 (after 1956). The variation of char was similar to BC, while nonhomologous growth was detected in char and soot (r = 0.29 and p > 0.05). The source apportionment showed that biomass burning for 71.52 ± 10.23% of char and promoted char sequestration. The contribution of fossil fuel combustion to soot (46.67 ± 14.07%) is much higher than char (28.48 ± 10.23%). Redundancy analysis confirmed that local anthropogenic activities significantly influenced BC burial and atmospheric transport from outside TP-regulated BC burial. The contribution of biomass and fossil fuels to nonsynchronous char and soot is conducive to understanding the anthropogenic effect on BC burial in the TP.

Polycyclic aromatic hydrocarbons in remote lakes from the Tibetan Plateau: Concentrations, source, ecological risk, and influencing factors.

Polycyclic aromatic hydrocarbons (PAHs) have received worldwide attention due to their potential teratogenic, persistent, and carcinogenic characteristics. In this study, the PAHs concentrations in two dated sediment cores taken from central Tibetan Plateau (TP) were analyzed to study the deposition history, potential sources, ecological risks, and influencing factors. Total concentration of PAHs (∑PAHs) ranged from 50.0 to 195 ng g-1 and 51.9-133 ng g-1 in sediments of Pung Co (PC) and Dagze Co (DZC), respectively. 2-3-ring PAHs were dominant in the two lake sediments, accounting for an average of 77.5% and 80.1%, respectively. The historical trends of ∑PAHs in the two lakes allowed to distinguish three periods, namely, relative stability before the 1950s, a gradual increase between the 1950s and the 1990s, and then a decline to the present-day. In addition, the trend in the concentration level of each PAH composition was consistent with ∑PAHs before the 1990s, while they exhibited different trends since the 1990s, which may be the result of a combination of anthropogenic activities and climate change in recent years, whereas before the 1990s the PAH profile was mainly influenced by atmospheric deposition. The results of source apportionment examined according to diagnostic ratios and positive matrix factorization were consistent and revealed that PAHs were primarily derived from biomass and coal combustion. Significant correlations between PAHs and organic carbon (OC) indicate that OC might be a key factor influencing the concentration of PAHs in sediments. The ecological risk assessment demonstrated that PAHs in TP sediments occurred at a low risk level. Results of this study could be helpful to develop a deeper insight into the deposition history of PAHs in remote lakes of the TP region and explore the response of these variations to climate change and human activities.

Coal combustion facilitating faster burial of char than soot in a plateau lake of southwest China.

Black carbon (BC) is a retarder in carbon cycle, and the proportion of char and soot in BC restricts the significance of BC as a sink in carbon cycle. Tracing the sources of char and soot is helpful for in-depth understanding the anthropogenic-driven burial and pattern of BC, and is crucial for regulating emissions of BC and impact of BC on carbon cycle/climate change. This study investigated source-driven BC via the concentration and δ13C of BC (char and soot) in a Plateau lake sediment. The burial rate of BC (mean: 6.42 ± 5.09 g m-2 yr-1) showed an increasing trend (3.7 times after 1977 compared with before), and the growth rate of char (4.1 times) was faster than soot (2.5 times). The source trace results, showing faster growth of coal combustion ratio in char (increased 21% after 1980 compared with before) than soot (13%), proved that coal combustion promoted faster growth of char in BC. Redundancy analysis confirmed that more low-temperature utilization of coal urged a stronger driving force for char than soot, which caused BC to have lower aromatic content and higher reactivity in organic carbon pool from the past to present, further impact the effects of BC on carbon cycle.

Source apportionment of polycyclic aromatic hydrocarbons (PAHs) in a sediment core from Lake Dagze Co, Tibetan Plateau, China: Comparison of three receptor models.

Receptor models are a useful tool for identifying sources of polycyclic aromatic hydrocarbons (PAHs) in multiple environmental media. In this study, three different receptor models (including the principal component analysis-multiple linear regression (PCA-MLR), positive matrix factorization (PMF), and Unmix models) were used to apportion the sources of 16 priority PAHs in a sediment core of Lake Dagze Co. The ∑PAHs (sum of all 16 measured PAHs) concentrations ranged from 51.89 to 132.82 ng/g with an average of 80.39 ng/g. The ∑PAHs were dominated by 2-3 ring PAHs, accounting for 80.12% on average, thereby indicating that they mainly originated from biomass and coal combustion and/or from long-range atmospheric transportation. The three models produced consistent source apportionment results. The greatest contributor to ∑PAHs was biomass combustion, followed by coal combustion, vehicle emissions, and petrogenic sources. Moreover, the temporal variation of the common sources was well-correlated among models. The multi-method comparison and evaluation results showed that all three models were useful tools for source apportionment of PAHs, with the PMF model providing better results than the PCA-MLR and Unmix models. The temporal trends of factor contributions were verified by PAHs with different ring numbers. Significant correlations were found between the simulated concentrations of each source factor and the PAHs with different ring numbers (P<0.01), except for the petrogenic source identified by the Unmix model (P>0.05). This study can provide useful information for further investigation of source apportionment of PAHs in the sediment cores.

Stable carbon isotopes trace the effect of fossil fuels on fractions of particulate black carbon in a large urban lake in China.

Black carbon (BC), the highly recalcitrant aromatic carbonaceous from the incomplete combustion of fossil fuel and biomass, is an important carbon sink in carbon cycle. Char and soot, the main components of BC, have significantly different origin and physicochemical characteristics (particle sizes and resultant transportability). The limited understanding of char and soot sources leads to poor insight into the effect of BC on carbon cycle. Sources of char and soot were investigated in this study using stable carbon isotopes to study the effect of BC on the organic carbon pool in a lake, thereby improving the knowledge of lacustrine carbon cycling. The concentration of BC in Taihu Lake ranged from 0.0 to 0.7 mg·L-1and accounted for 10.9 ± 4.7% of the particulate organic carbon. The spatial-mean δ13C values of BC, char, and soot were -23.2 ± 2.0‰, -23.5 ± 2.2‰, and -22.9 ± 1.6‰, respectively. The BC in water was primarily derived from fossil fuels (66.0 ± 9.3%), with liquid fossil fuel accounting for 48.2 ± 13.2% of the BC. The contribution of liquid fossil fuel to soot (49.3%) was much higher than that to char (36.1%); correspondingly, the contributions of biomass and coal to soot (29.2% and 21.5%) were lower than those to char (38.1% and 25.8%). The contribution of liquid fossil fuel combustion to organic carbon (OC), char, and soot gradually increased from 31.9% to 49.3%. Biomass and coal combustion primarily contributed to char (38.1% and 25.8%) and OC (37.5% and 30.6%). The source apportionment of BC, char, and soot revealed the influence of anthropogenically driven BC, char, and soot on the lake and, by extension, to the global carbon cycle.

Spatial variation of particulate black carbon, and its sources in a large eutrophic urban lake in China.

Black carbon (BC), characterized by high aromaticity and stability, has been recognized as a substantial fraction of the carbon pool in soil and sediment. The effect of BC on the particulate organic carbon (POC) pool in lake water, which is an important medium of carbon transmission and transformation, has not been thoroughly studied. The investigations of BC composition and distribution, POC, polycyclic aromatic hydrocarbons (PAHs), and stable carbon and nitrogen isotopes were conducted in a eutrophic urban lake, Taihu Lake, which is the third largest freshwater lake in China. The results indicate that the BC is composed of 55 ± 12% char and 45 ± 12% soot and accounted for 12 ± 6% of POC (the maximum value is 31%). The comparatively high levels of BC and char are distributed in the northern Taihu Lake, especially in Meiliang Bay (0.72 ± 0.38 mg L-1 and 0.45 ± 0.24 mg L-1). The distribution of soot presents a declining trend from the lakeshore to the central lake, particularly in the northern, western, and southern lakes. Source apportionment results from positive matrix factorization of PAHs suggest that consumption of fossil fuel (79 ± 20%) is the dominant source of BC, which agrees with the low ratio of char/soot (1.41 ± 0.71) and relatively depleted δ13C. The covariation of BC and PAHs and terrestrial dissolved organic carbon indicate that the effect of terrestrial input significantly regulates the distribution of BC in Taihu Lake, which is reflected in the high BC value along the lakeshore.

Anthropogenic-Driven Alterations in Black Carbon Sequestration and the Structure in a Deep Plateau Lake.

The continuous flux of organic carbon (OC) from terrestrial ecosystems into inland water is an important component of the global carbon cycle. The buried OC pool in inland water sediments is considerable, and black carbon (BC) is a significant contributor to this OC pool because of the continuous growth in BC emissions. Therefore, determining the effect of BC on total OC burial and variations in the structure of BC during the burial process will contribute significantly to our understanding of lacustrine carbon cycling. This study investigated BC burial and its structural variations in response to anthropogenic drivers using four dated sedimentary cores from a deep plateau lake in China. The BC burial rate rose from 0.96 ± 0.64 g·m-2·y-1 (mean of sedimentary cores pre-1960s) to 4.83 ± 1.25 g·m-2·y-1 (after 2000), which is a 5.48 ± 2.12-fold rise. The increase of char was similar to those of BC. The growth rate of soot was 7.20 ± 4.30 times, which is higher than that of BC and char, increasing from 0.12 ± 0.08 to 0.64 ± 0.23 g·m-2·y-1. There was a decreasing trend in the ratio of char and soot at a mean rate of 62.8 ± 6.46% (excluding core 3) in relation to increased fossil fuel consumption. The contribution of BC to OC burial showed a significant increasing trend from the past to the present, particularly in cores 3 and 4, and the mean contribution of the four cores was 11.78 ± 2.84%. Source tracer results from positive matrix factorization confirmed that the substantial use of fossil fuels has promoted BC burial and altered the BC structure. This has resulted in BC with a higher aromatic content in the lake sediment, which exhibits reduced reactivity and increased stability. The strong correlation between BC and allochthonous total OC indicates that the input pathways of the buried BC in this plateau lake sediment were terrestrial surface processes and not atmospheric deposition.