Yu-Feng Guan

Organochlorine pesticides and polychlorinated biphenyls in riverine runoff of the Pearl River Delta, China: assessment of mass loading, input source and environmental fate.

A large-scale sampling program was conducted to simultaneously collect water samples at the eight major riverine runoff outlets of the Pearl River Delta (PRD), South China to assess the importance of riverine runoff in transporting anthropogenic pollutants from terrestrial sources to the coastal ocean. The concentrations of Sigma21OCPs (sum of 21 OCP components) and Sigma20PCBs (sum of 20 PCB congeners) were 2.57-41.2 and 0.12-1.47 ng/L, respectively. Compositional distributions of DDTs suggested the possibility of new input sources in the study area, but contributions from dicofol seemed considerably low. The annual inputs of Sigma21OCPs and Sigma20PCBs were 3090 and 215 kg, with those of total HCHs and DDTs being 1110 and 1020 kg, respectively. A mass balance consideration indicated that riverine runoff is the major mode carrying OCPs from the PRD to the coastal ocean, and the majority of OCPs is further dissipated to open seas.

Sediment Records of Polycyclic Aromatic Hydrocarbons (PAHs) in the Continental Shelf of China: Implications for Evolving Anthropogenic Impacts

Sources, compositions, and historical records of polycyclic aromatic hydrocarbons (PAHs) in sediment cores collected from the Yellow Sea and the South China Sea were analyzed to investigate the influence of anthropogenic activities. The occurrence of PAHs was mainly derived from various combustion sources, especially the combustion of biomass and domestic coal. Uniform composition of sedimentary PAHs (52-62% of phenanthrene, benzo[b]fluoranthene, indeno[1,2,3-cd]pyrene, and benzo[g,h,i]perylene) suggested air-borne mixtures intractable to degradation. The concentrations of the sum of 15 PAHs (16 priority pollutants designed by the United States Environmental Protection Agency minus naphthalene; designed as Σ(15)PAH) in Yellow Sea sediment cores were generally higher than those in the South China Sea. The profiles of Σ(15)PAH concentrations recorded in the sediment cores closely followed historical socioeconomic development in China. In general, Σ(15)PAH concentrations started to increase from the background pollution level posed by agricultural economy at the turn of 20th century. In addition, a Σ(15)PAH concentration reduction was observed during the Chinese Civil War (1946-1949) and Great Cultural Revolution (1966-1976), suggesting them as setbacks for economic development in Chinese history. Increasing PAH emissions as a result of increasing coal combustion associated with the rapid urbanization and industrialization since the implementation of the Reform and Open Policy (since 1978) accounted for the fast growth of Σ(15)PAH concentrations in sediment cores. The decline of Σ(15)PAH concentrations from subsurface maximum until sampling time was inconsistent with current-day economic development in China, and may possibly suggest emission reductions due to decreasing proportional use of domestic coal and increasing consumption of cleaner energies (natural gas and liquefied petroleum gas).

Occurrence of Polybrominated Diphenyl Ethers in Air and Precipitation of the Pearl River Delta, South China: Annual Washout Ratios and Depositional Rates

On the basis of a one-year (from October 2006 to September 2007) sampling campaign, 34 air samples and 23 bulk precipitation samples were collected in the Pearl River Delta (PRD) in southern China and analyzed for polybrominated diphenyl ethers (PBDEs). Fifteen tri- to deca-BDE congeners (sum of which is defined as Sigma15PBDE) were detected in more than 70% of the samples. In three urban-rural regions, Sigma15PBDE concentrations ranged from 77 to 372 pg/m3 in air (particulate + vapor) and 1.98 to 15.5 ng/L in rain (particle+dissolved) from Dongguan, from 195 to 1450 pg/m3 in air and 4.71 to 17.2 ng/L in rain from Shunde, and from 23.7 to 148 ng/L in rain from Guangzhou. Among the BDE congeners, BDE-209 was the predominant component. Linear correlations between the gas-particle partition coefficients (Kp) and the subcooled vapor pressures (P(O/L)) of individual BDE congeners were observed for both the wet and dry seasons, but the slopes (-0.572 to -0.525) of the fitted equations all substantially deviated from equilibrium condition (slope = -1). The total washout ratio by bulk rainfalls was determined to be 2 x 103 for tri-BDEs and 6 x 104 for BDE-209. The estimated annual dry and wet depositional rates were 6720 and 2460 kg/yr, respectively, for BDE-209, and 7270 and 2940 kg/yr for Sigma15PBDE in the PRD, indicating a dominant pathway for PBDEs input into the PRD soil and aquatic environments.

Polycyclic aromatic hydrocarbons (PAHs) in continental shelf sediment of China: Implications for anthropogenic influences on coastal marine environment

Sediments collected from the continental shelf of China, embracing Yellow Sea, inner shelf of the East China Sea (ECS), and the South China Sea (SCS), were analyzed for polycyclic aromatic hydrocarbons (PAHs). The concentrations of anthropogenic PAHs (Σ(18)PAH) were 27-224 ng/g dry weight, with an average of 82 ng/g. Sedimentary PAHs in the continental shelf off China were mainly derived from mixed residues of biomass, coal, and petroleum combustion. Fluvial transport and atmospheric deposition mainly accounted for sediment PAHs in the ECS inner shelf and Yellow Sea (and the SCS), respectively. Furthermore, statistically higher levels of Σ(18)PAH (28-224 ng/g; mean 110 ng/g) in the Yellow Sea sediment than in the SCS sediment (28-109 ng/g; mean 58 ng/g) were probably resulted from higher PAH emissions from coke industry and domestic coal combustion in North China than in South China.

Fate of polybrominated diphenyl ethers in the environment of the Pearl River Estuary, South China

Ninety-six riverine runoff samples collected at eight major outlets in the Pearl River Delta (PRD), South China, during 2005-2006 were analyzed for 17 brominated diphenyl ether (BDE) congeners (defined as Sigma17PBDE). Fourteen and 15 congeners were detected, respectively, in the dissolved and particulate phases. These data were further used to elucidate the partitioning behavior of BDE congeners in riverine runoff. Several related fate processes, i.e. air-water exchange, dry and wet deposition, degradation, and sedimentation, within the Pearl River Estuary (PRE), were examined to estimate the inputs of Sigma10PBDE (sum of the target BDE congeners, BDE-28, -47, -66, -85, -99, -100, -138, -153, -154, and -183) and BDE-209 from the PRD to the coastal ocean based on mass balance considerations. The results showed that annual outflows of Sigma10PBDE and BDE-209 were estimated at 126 and 940 kg/year, respectively from the PRE to coastal ocean. Besides sedimentation and degradation, the majority of Sigma10PBDE and BDE-209 discharged into the PRE via riverine runoff was transported to the coastal ocean.

Polycyclic aromatic hydrocarbons in upstream riverine runoff of the Pearl River Delta, China: An assessment of regional input sources

Water samples collected from upstream tributaries of the Pearl River Delta (PRD) and from locations within the PRD (South China) were analyzed for 27 polycyclic aromatic hydrocarbons (PAHs). Average concentrations (aqueous plus particulate) of total 27 PAHs (Σ(27)PAH), 16 priority PAHs designated by the United States Environmental Protection Agency (USEPA) except naphthalene (Σ(15)PAH), and the seven carcinogenic PAHs (Σ(7)PAH) classified by the USEPA were 260 ± 410, 130 ± 310, and 15 ± 12 ng/L, respectively. Riverine PAHs were predominantly generated from coal and vegetation combustion, coke production, vehicle exhausts, and petroleum residues, accounting for 28%, 25%, 22% and 21%, respectively, on average. Upstream riverine fluxes of Σ(27)PAH and Σ(15)PAH amounted to 38.9 and 12.9 tons/year, respectively. The net contributions of Σ(27)PAH and Σ(15)PAH from sources within the PRD were estimated at 21.4 and 21.0 tons/year, respectively.

Occurrence, bioaccumulation and potential sources of polybrominated diphenyl ethers in typical freshwater cultured fish ponds of South China

To determine the potential input sources of polybrominated diphenyl ethers (PBDEs) to fish farming environments in South China, samples of seven various environmental matrices were collected from October 2006-September 2007. Tri- to deca-BDEs were detected in all samples analyzed, with mean concentrations (+ or - standard deviations) at 5.7 + or - 3.6 ng/L in pond water, 15 + or - 11 ng/g dry wt. in pond sediment, 12 + or - 3.8 ng/g dry wt. in bank soil, 21 + or - 20 ng/g lipid wt. in fish, and 93 + or - 62 ng/g lipid wt. in fish feeds. In addition, BDE-209 was the major constituent in all samples except fish and BDE-47 was predominant in fish samples. Relatively high abundances of BDE-49 were detected in all the samples compared to those in the penta-BDE technical products. Several bioaccumulation factors were evaluated. Finally, statistical analyses suggested that fish feed, as well as pond water at a lesser degree, may have been the major source of PBDEs in freshwater farmed fish.

Use of aliphatic hydrocarbons to infer terrestrial organic matter in coastal marine sediments off China.

Sediment samples from the marine systems along the coast of China, covering Yellow Sea, inner shelf of the East China Sea (ECS) and the South China Sea (SCS), were analyzed for n-alkanes and organic carbon. The concentrations of Σn-C(15-35) were 120-1680 ng g(-1) dry weight with an average of 560 ng g(-1). Short-chain n-alkanes (<C(21)) in Yellow Sea and the SCS were derived from mixed bacteria and planktonic sources, while those in the ECS inner shelf were mainly of planktonic sources. Long-chain n-alkanes (>C(21)) were mainly derived from terrestrial higher plants. Organic carbon deposited into Yellow Sea and Southeast Hainan within the SCS was mainly of terrestrial (13-110%; mean: 58%) and marine (48-110%; mean: 86%) sources, respectively. On the other hand, organic carbon accumulated in the SCS adjacent to the Pearl River Estuary was derived from both terrestrial and marine sources.

Sedimentary record of polycyclic aromatic hydrocarbons in a sediment core from a maar lake, Northeast China: evidence in historical atmospheric deposition

A maar lake is an excellent ecosystem to study the atmospheric deposition of pollutants, as its contaminants are primarily by atmospheric deposition. In this study, a sediment core from Sihailongwan Maar Lake, Northeast China, was collected and the historical atmospherically deposited polycyclic aromatic hydrocarbons (PAHs) were analyzed. The concentrations of TPAHs (the sum of the US EPA proposed 16 priority PAHs, excluding naphthalene and pyrene) ranged from 473.9 to 2289 ng g(-1) with a slow increasing stage in the deeper sediments and a sharp increasing stage in the upper sediments. The input rate of TPAHs, especially that of PAH(9) (the sum of fluoranthene, benzo(a)anthracene, chrysene, benzo(b)fluoranthene, benzo(k)fluoranthene, benzo(a)pyrene, indeno(1,2,3-cd)pyrene, dibenzo(ah)anthrathene, and benzo(ghi)perylene), correlated well to the Chinese historical socioeconomic data. This indicates that sediment PAHs were mainly derived from human activities and PAH(9) can be regarded as a better indicator of the local socioeconomic development. Source identification suggested that PAHs were originated primarily from mixed sources (e.g., coal and biomass burning and petroleum combustion), except for perylene which was mostly of diagenetic origin. In addition, the down-core PAHs profile clearly illustrated that PAHs sources in Northeast China experienced a transformation from low- and moderate temperature to high-temperature combustion processes, especially after the late 1980s. Additionally, an ecological risk assessment using two redefined biological thresholds (TEQ(ERL) and TEQ(ERM)) indicated that most of the PAHs measured in the present sediment core would not cause an immediate toxic effect; only FLU and PHEN are a potential source of concern for biological impairment.

Occurrence and mass loadings of n-Alkanes in riverine runoff of the Pearl River Delta, South China: Global implications for levels and inputs†

Riverine runoff samples were collected monthly from March 2005 to February 2006 from the eight major outlets of the Pearl River Delta (PRD), South China, and analyzed to obtain the concentrations of n-alkanes in both the filtrate and particulate phases. The average concentrations of Sigma(C15-C34) (i.e., sum of C15 to C34 normal alkanes) ranged from 0.06 to 2.97 microg/L (mean, 0.64 microg/L) in filtrate samples and from 1.00 to 98.8 microg/g (average, 19.8 microg/g dry weight) in particulate samples. Compared to results from around the world, the levels of hydrocarbon compounds in the PRD were at the high end of the global range. Evaluation of compositional indices of n-alkanes indicated that petroleum-related sources are the main contributor of n-alkanes found in the PRD, with minor contributions from high plant wax. Regression analyses appeared to suggest that n-alkanes are transported into the aquatic environment of the PRD via various pathways, and the transport mechanisms also are considerably influenced by the complex hydrologic conditions in the PRD. The annual riverine input of Sigma(C15-C34) from the PRD to the coastal ocean was 360 tons/year, or the equivalent of approximately 8,800 tons/year of petroleum hydrocarbons. The emission of Sigma(C15-C34) from all sources in the PRD was estimated at 39,000 tons/year, or 2.4 g/day per capita. Overall, the PRD contributes approximately 0.2% of the annual global input of n-alkanes to the coastal oceans, similar to the contributions of polycyclic aromatic hydrocarbons, further indicating that the PRD has been a significant source of hydrocarbon contamination to the global coastal marine environment.