Effects of Temperature and DC Electric Fields on Perfluorooctanoic Acid Sorption Kinetics to Activated Carbon.

Sorption to activated carbon is a common approach to reducing environmental risks of waterborne perfluorooctanoic acid (PFOA), while effective and flexible approaches to PFOA sorption are needed. Variations in temperature or the use of electrokinetic phenomena (electroosmosis and electromigration) in the presence of external DC electric fields have been shown to alter the contaminant sorption of contaminants. Their role in PFOA sorption, however, remains unclear. Here, we investigated the joint effects of DC electric fields and the temperature on the sorption of PFOA on activated carbon. Temperature-dependent batch and column sorption experiments were performed in the presence and absence of DC fields, and the results were evaluated by using different kinetic sorption models. We found an emerging interplay of DC and temperature on PFOA sorption, which was linked via the liquid viscosity (η) of the electrolyte. For instance, the combined presence of a DC field and low temperature increased the PFOA loading up to 38% in 48 h relative to DC-free controls. We further developed a model that allowed us to predict temperature- and DC field strength-dependent electrokinetic benefits on the drivers of PFOA sorption kinetics (i.e., intraparticle diffusivity and the film mass transfer coefficient). Our insights may give rise to future DC- and temperature-driven applications for PFOA sorption, for instance, in response to fluctuating PFOA concentrations in contaminated water streams.

Structure-dependent degradation of phthalate esters with persulfate oxidation activated by thermal in soil.

Phthalate esters (PAEs) have become one of the most concerned emerging organic pollutants in the world, due to the toxicity to human health, and hard to remove it efficiently. In this study, the degradation performance of DBP and DEHP in the soil by water bath heating activated sodium persulfate (PS) method under different factors were studied, in which the degradation rate of DBP and DEHP were improved with the increasing of temperature, PS concentration and water/soil ratio, and higher diffusion efficiency treatments methods, due to the improved mass transfer from organic phase to aqueous media. However, the degradation rate of DEHP was much lower than that of DBP, because DEHP in the soil was more difficult to contact with SO4•- for reaction on soil surface, and the degradation rate of PAEs in soil was significantly lower than that in water. Redundancy analysis of degradation rate of DBP and DEHP in water demonstrated that the key factors that determine the degradation rate is time for DBP, and cosolvent dosage for DEHP, indicating that the solubility and diffusion rate of PAEs from soil to aqueous are predominance function. This study provides comprehensive scenes in PAEs degradation with persulfate oxidation activated by thermal in soil, reveal the difference of degradation between DBP and DEHP is structure-dependent. So that we provide fundamental understanding and theoretical operation for subsequent filed treatment of various structural emerging pollutants PAEs contaminated soil with thermal activated persulfate.

Heat and mass transfer induced by alternating current during desorption of PAHs from soil using electrical resistance heating.

The transfer of heat and contaminants by alternating current (AC) and the removal mechanism of polycyclic aromatic hydrocarbons (PAHs) in electrical resistance heating (ERH) need further study. The main factors affecting heat transfer and water evaporation in the ERH experiment were studied, and the desorption efficiency, temporal and spatial distribution and kinetic behavior under various conditions were analyzed. The results suggested that moisture content was a necessary condition to ensure effective heating of soil, and soil moisture content above 30% was recommended. Higher voltage intensity and/or ion concentration meant stronger input power, resulting in the rapider heating process and the shorter the boiling time. At a low desorption temperature (about 100°C), the Phe desorption mainly depended on the volatilization of surface Phe and the co-boiling of Phe-water. In ERH, the participation of AC would accelerate the diffusion of pollutants from the internal pores of soil particles and their redistribution with water phase, thus improving the Phe removed by co-boiling. It was noteworthy that AC just greatly promoted solid-liquid mass transfer, but it hardly promoted desorption directly, and the removal still depended on Phe-water co-boiling. The Phe desorption efficiency could be significantly improved from 14.0~18.4% to 59.6~70.8% under the combined action of current strengthening Phe diffusion and co-boiling. Thermogravimetric and product analysis confirmed that no new organic matter was generated, but only Phe entered the gas phase through phase change.

Feasibility of using Vis-NIR spectroscopy and PXRF spectrometry to estimate regional soil cadmium concentration.

Conventionally, soil cadmium (Cd) measurements in the laboratory are expensive and time-consuming, involving complex processes of sample preparation and chemical analysis. This study aimed to identify the feasibility of using sensor data of visible near-infrared reflectance (Vis-NIR) spectroscopy and portable X-ray fluorescence spectrometry (PXRF) to estimate regional soil Cd concentration in a time- and cost-saving manner. The sensor data of Vis-NIR and PXRF, and Cd concentrations of 128 surface soils from Yunnan Province, China, were measured. Outer-product analysis (OPA) was used for synthesizing the sensor data and Granger-Ramanathan averaging (GRA) was applied to fuse the model results. Artificial neural network (ANN) models were built using Vis-NIR data, PXRF data, and OPA data, respectively. Results showed that: (1) ANN model based on PXRF data performed better than that based on Vis-NIR data for soil Cd estimation; (2) Fusion methods of both OPA and GRA had higher predictive power (R2) = 0.89, ratios of performance to interquartile range (RPIQ) = 4.14, and lower root mean squared error (RMSE) = 0.06, in ANN model based on OPA fusion; R2 = 0.88, RMSE = 0.06, and RPIQ = 3.53 in GRA model) than those based on either Vis-NIR data or PXRF data. In conclusion, there exists a great potential for the combination of OPA fusion and ANN to estimate soil Cd concentration rapidly and accurately.

Mechanisms of heating-electrokinetic co-driven perfluorooctanoic acid (PFOA) adsorption on zeolite.

Slow release of emerging contaminants limits their accessibility from soil to pore water, constraining the treatment efficiency of physio-chemical treatment sites. DC fields mobilize organic contaminants and influence their interactions with geo-matrices such as zeolites. Poor knowledge, however, exists on the joint application of heating and electrokinetic approaches on perfluorooctanoic acid (PFOA) transport in porous media. Here, we investigated electrokinetic PFOA transport in zeolite-filled percolation columns at varying temperatures. Variations of pseudo-second-order kinetic constants (kPSO) were correlated to the liquid viscosity variations (η) and elctroosmotic flow velocities (vEOF). Applying DC fields and elevated temperature significantly (>37%) decreased PFOA sorption to zeolite. A good correlation between η, vEOF, and kPSO was found and used to develop an approach interlinking the three parameters to predict the joint effects of DC fields and temperature on PFOA sorption kinetics. These findings may give rise to future applications for better tailoring PFOA transport in environmental biotechnology.

Revealing the Mechanism of Dioxin Formation from Municipal Solid Waste Gasification in a Reducing Atmosphere.

Gasification is an effective technology for the thermal disposal of municipal solid waste (MSW) with lower dioxin emission compared to the prevailing incineration process. Nevertheless, the mechanism of dioxin formation in the reducing atmosphere during the gasification process was seldomly explored. Herein, the effects of the atmosphere, temperature, and chlorine source were systematically investigated in terms of dioxin distribution. With CO2 and H2O as gasification agents, a reducing reaction atmosphere was formed with abundant H2 which effectively suppressed the generation of C-Cl, contributing to a substantial decrease of dioxin concentration by ∼80% compared to the incineration process. The formation of dioxin was favored at temperatures below 700 °C with its peak concentration achieved at 500 °C. It was unveiled that inorganic chlorine played a dominant role in the reducing atmosphere, with a lower proportion of C-O-C/O-C═O on residual slag compared to an oxidizing atmosphere. Additionally, the generated H2 reduced the concentration of dioxins by attacking C-Cl and inhibiting the crucial Deacon reaction for dioxin formation, validated by density functional theory calculation. Eventually, the formation route paradigm and the reaction mechanism of dioxin formation from MSW gasification were revealed, facilitating and rationally guiding the control of dioxin emission.

Biochar facilitated bacterial reduction of Cr(VI) by Shewanella Putrefaciens CN32: Pathways and surface characteristics.

Biochar can facilitate the microbial reduction of various pollutants in soil and groundwater environments, but its impact on Cr(VI) reduction by dissimilatory metal reducing bacteria (DMRB) remains to be systematically investigated. In this study, we prepared biochars at 500 °C and 700 °C from wheat straw and grass, and investigated the impact of these biochars on Cr(VI) reduction by a model DMRB, Shewanella Putrefaciens CN32 (CN32). Pristine biochars abiotically reduced Cr(VI), which decreased the concentration and toxicity of chromium to CN32 cells, and brought about higher overall Cr(VI) removal extent after CN32 were added sequentially; on the other hand, no enhancement effect were observed when biochars and CN32 were added simultaneously. Further tests between biologically reduced biochars and Cr(VI) revealed that the reaction rates between bioreduced biochars and Cr(VI) are relatively sluggish compared to that of direct Cr(VI) reduction by CN32, which prohibited biochars from directly accelerating the Cr(VI) reduction by CN32 in simultaneous-addition scenario. The relative importance of biochars' surface functional groups and surface areas on their reactivities towards Cr(VI) reduction were also investigated. This study deepened our understanding towards the role of biochar played during bacterial Cr(VI) reduction and could potentially contribute to optimizing the biochar-based Cr(VI) bioremediation strategies.

Modification of activated carbon using urea to enhance the adsorption of dioxins.

Activated carbon is commonly used to remove dioxins from flue gas via adsorption. Improving the targeted adsorption capacity of activated carbon for dioxins can reduce the consumption of adsorbents and help achieve emission standards for target pollutants. Here, commercial coal-based activated carbon was used as a raw material and modified by urea impregnation along with treatment at high temperature under a nitrogen atmosphere. It was found that modification with urea effectively improved the pore structure of activated carbon while incorporating a certain amount of nitrogen. The best modification effect was achieved at a modification temperature of 600 °C, an impregnation ratio of urea to activated carbon of 1:1, and with high-temperature treatment for 2 h. The mesopore volume of the modified activated carbon (AC600) reached 0.38 cm3/g, accounting for 57.58% of the total pore volume. With an impregnation ratio of urea to activated carbon of 1:1, high-temperature treatment for 2 h, and a modification temperature of 800 °C, a certain amount of nitrogen was introduced into the carbon rings to form a modified activated carbon (AC800) rich in pyridine and pyrrole groups (atomic percentage = 4.84%). The activated carbon modified by urea and the unmodified activated carbon were subsequently selected for dioxin adsorption experiments using a dioxin generation and adsorption system. AC600 showed the highest adsorption efficiency for dioxins, reaching 97.65%, based on toxicity equivalents. Although AC800 has poor pore properties, it has more pyridine and pyrrole groups than AC600. Consequently, the efficiency of AC800 at adsorbing low-concentration dioxins reached 85.24% based on toxicity equivalents. Overall, this study describes two mechanisms for effectively modifying activated carbon with urea based on (1) optimizing the pore structure of activated carbon and (2) incorporating nitrogen.

Application of microbial fuel cell technology to the remediation of compound heavy metal contamination in soil.

Exploring the removal rules of MFC on composite heavy metal pollution is very important for the future development and field application of MFC. We constructed a three-chamber soil MFC and the results showed that with the gradual deterioration of soil heavy metal contamination from single heavy metal to metals in different oxidation states (e.g., copper (II), lead (II), and chromium (III) compounds), the internal resistance of the soil MFC increased by 2.16-2.71 times, which significantly inhibited the power production performance of the MFC. After 59 days of remediation, the migration removal efficiencies of total Cu, total Cr and total Pb from the soil under composite conditions were 36.69%, 52.35% and 19.67%, respectively. The main removal mechanisms included both electromigration and diffusion, where electromigration contributed 74.41%, 31.48% and 97.67% to the removal of total Cu, Cr and Pb, respectively. The removal of composite heavy metals was affected by adsorption-desorption competition and synergism. The competition of Pb for specific adsorption sites in soil leads to the increase of mobility of Cr and Cu, which is conducive to migration and removal. The migration of Cu and Pb ions to the cathode inhibited the diffusion of Cr to the anode; however, it drove the synergistic migration of Pb ions to the cathode. For the heavy metals migrated from the soil into the catholyte, only Cu2+ with high redox potential is reduced to copper at the cathode.

Enhanced Adsorption of Sulfonamides by Attapulgite-Doped Biochar Prepared with Calcination.

The extensive use of sulfonamides seriously threatens the safety and stability of the ecological environment. Developing green inexpensive and effective adsorbents is critically needed for the elimination of sulfonamides from wastewater. The non-modified biochar exhibited limited adsorption capacity for sulfonamides. In this study, the attapulgite-doped biochar adsorbent (ATP/BC) was produced from attapulgite and rice straw by calcination. Compared with non-modified biochar, the specific surface area of ATP/BC increased by 73.53−131.26%, and the average pore width of ATP/BC decreased 1.77−3.60 nm. The removal rates of sulfadiazine and sulfamethazine by ATP/BC were 98.63% and 98.24%, respectively, at the mass ratio of ATP to rice straw = 1:10, time = 4 h, dosage = 2 g∙L−1, pH = 5, initial concentration = 1 mg∙L−1, and temperature = 20 °C. A pseudo-second-order kinetic model (R2 = 0.99) and the Freundlich isothermal model (R2 = 0.99) well described the process of sulfonamide adsorption on ATP/BC. Thermodynamic calculations showed that the adsorption behavior of sulfonamides on the ATP/BC was an endothermic (ΔH > 0), random (ΔS > 0), spontaneous reaction (ΔG < 0) that was dominated by chemisorption (−20 kJ∙mol−1 > ΔG). The potential adsorption mechanisms include electrostatic interaction, hydrogen bonding, π−π interaction, and Lewis acid−base interactions. This study provides an optional material to treat sulfonamides in wastewater and groundwater.

Spatial Distribution and Assessment of the Human Health Risks of Heavy Metals in a Retired Pharmaceutical Industrial Area, Southwest China.

Heavy metals pollution in pharmaceutical industries received increasing attention. A total of 94 soil samples were collected in this study. Results showed the mean contents of Hg, Cd, As, Pb, Ni and Cu were 0.21, 0.26, 9.59, 55.06, 51.52 and 50.81 mg·kg-1, respectively. The spatial distribution of metals in topsoil largely attributed to the pharmaceutical production process. The distribution of Hg and As were related to the production of medical absorbent cotton. While Ni was related to the fuel supply of Ni-rich coal. Cr, Cu and Pb mainly distributed in the process which they were used as catalysts. The vertical migration of metals was complex in soil. To a great extent, it was related to the texture of the soil and the properties of metals in this filed. The total non-cancer and cancer human health risk were within the limits of USEPA (10-6 a-1). This demonstrated the health risks of individual's exposure to heavy metals in this factory was acceptable.

Enhancing remediation of PAH-contaminated soil through coupling electrical resistance heating using Na2S2O8.

Soil polycyclic aromatic hydrocarbons (PAHs) contamination caused by factory relocations is a serious environmental issue across the world. Electrical resistance heating (ERH) and chemical oxidation are two promising in-situ methods for treating volatile and semi-volatile organic pollutants in contaminated soil. Coupling of ERH and chemical oxidation technologies to improve the remediation efficiency for PAH-contaminated soil was estimated in this study. PAH removal ratio in contaminated soils using ERH treatment were significantly negatively correlated with the boiling point of the pollutants (P = 0.002), and 21.63% (DBA high boiling point) to 71.53% (Nap low boiling point) of PAHs in the contaminated soil were removed in 120 min. With oxidant Na2S2O8 coupling, the removal ratio were increased as more oxidant was added. For one Phe, 35.90% was removed by ERH treatment and increased to 52.90% and 79.42% when 0.05 or 2.5 mmol/g oxidant was added, respectively. PAHs with higher boiling points had more obvious removal ratio, such as Bap, which increased from 23.50% to 85.47% when coupling ERH with Na2S2O8, and Phe which increased from 35.90% to 79.42%. Relationships between boiling points and PAH removal ratio changed with coupled oxidants, indicating a change of mechanism from volatilization to coupling effects of volatilization and oxidation with the introduction of Na2S2O8. A dynamic experiment showed that Na2S2O8 can accelerate 45.50% of the treatment process. The results of this research demonstrated a novel, cost-effective coupling approach for remediating soil contaminated by organic pollutants.

Spatial distribution and assessment of the human health risks of heavy metals in a retired petrochemical industrial area, south China.

Petrochemical industries are widely distributed in China. As a negative consequence, heavy metals in petrochemical area can result in soil contamination. However, the relevant research of heavy metals contamination in petrochemical area was few. In this study, a total of 103 topsoil samples (<20 cm) and 25 profile soil samples were collected and examined in a retired petrochemical industrial area, South China. The results showed the mean contents of Hg, Cd, As, Pb, Ni and Cu were 0.18, 0.69, 16.22, 47.24, 31.62 and 93.06 mg kg-1, respectively. The spatial distribution of six metals in topsoil was largely attributed to the industrial activities during the petroleum refining and transshipment process. Ni was the main pollutant in the petroleum refining process. While, the contamination of other metals mainly were caused by the leakage of the oil during transshipment. The migration of six metals to subsoil layers was also observable. In accordance, Hg, Cd, As, Pb, Cu, and Ni dropped by 95.02, 71.91, 89.45, 90.88, 99.22, and 65.07%, respectively, compared to their contents in topsoil. The contamination of the heavy metals was mainly caused during the process of petroleum refining and transshipment. The distribution of heavy metals in the factory was mainly affected by the industrial activities or the lateral infiltration of Lianhuashan River. Soil ingestion was the primary pathway for children and adults exposure to heavy metals. The total non-cancer human health risk induced by heavy metals was within the limit of USEPA (10-6 a-1). While the cancer risks alone induced by As through soil ingestion to children was 1.14 × 10-6 a-1, which exceeded the limit of USEPA. This study indicated that not only petroleum hydrocarbon but also heavy metals can cause soil contamination in a retired petrochemical industrial area, which provides a novel cognition. Altogether, measures should be taken in practice to substantially improve the soil quality in petrochemical industrial area.

Coupled photocatalytic-bacterial degradation of pyrene: Removal enhancement and bacterial community responses.

Polycyclic aromatic hydrocarbons (PAHs) are a class of pollutants that ubiquitously present in environment and hard to be degraded by microorganisms. Herein, we reported a novel photocatalytic-bacterial coupled removal system to treat PAH-polluted water. Using pyrene as the model pollutant, we demonstrated that the removal percentage of different groups was in order: 63.89% ± 1.03% (Vis-Biological) > 61.27% ± 1.08% (UV-Biological) > 59.58% ± 1.15% (UV) > 57.41% ± 1.13% (Vis) > 6.65% ± 0.72% (Biological) > 1.70% ± 0.34% (Control), showing the coupled system significantly improved the removal percentage of pyrene. Additionally, we observed that the coupled system driven by visible light showed higher removal percentage than UV light, exhibiting a good potential for future application. Sequencing analysis of 16S rRNA genes showed that alpha diversity (richness, evenness and diversity) got promoted and data of the relative abundance showed that Pseudomonadaceae was substituted as the dominant bacteria for Planococcaceae, with some other functional bacteria quickly acclimatizing in the bacterial community. Difference analysis indicated that over half of top fifteen genera were generally different significantly (p < 0.001) among two different samples, and UV light altered structure and composition of bacterial community more than visible light. Functional features' change suggested that the bacterial community not only protected itself but also participated in degrading pyrene. Overall, our study offered a new method for PAH degradation and contributed to further understanding of coupled catalytic-bacterial degradation processes.

Properties of hydrochars derived from swine manure by CaO assisted hydrothermal carbonization.

The hydrochars derived from swine manure were prepared by CaO assisted hydrothermal carbonization (HTC), and their properties were investigated for the first time. The results showed that the pH and yield of the hydrochar were largely increased by CaO addition. HTC of swine manure increased the phosphorus (P) content in the hydrochar, and appropriately 100% of P as apatite-P was enriched in the hydrochar by CaO assisted HTC. Additionally, the CaO addition during HTC improved the porosity of the hydrochar. The FTIR analysis revealed that substantial functional groups were present on the surface of the hydrochar, indicating the facilitated exchange between the hydrochar and hydrophilic soil when the hydrochar was used for soil amendment. This study demonstrated that CaO assisted HTC was a novel strategy to quickly convert swine manure to the promising soil amendment especially for acidic soils.

Analysis of influencing factors on public perception in contaminated site management: Simulation by structural equation modeling at four sites in China.

Public perception towards contaminated site management, a not readily quantifiable latent parameter, was linked through structural equation modeling in this paper to 22 measurable/observable manifest variables associated with the extent of information dissemination and public knowledge of soil pollution, attitude towards remediation policies, and participation in risk mitigation processes. Data obtained through a survey of 412 community residents at four remediation sites in China were employed in the model validation. The outcomes showed that public perception towards contaminated site management might be explained through selected measurable parameters in five categories, namely information disclosure, knowledge of soil pollution, expectations of remediation and redevelopment outcomes, public participation, and site policy, along with their interactions. Among these, information dissemination and attitude towards management policies exhibited significant influence in promoting positive public perception. Based on these examples, responsible agencies therefore should focus on public accessibility to reliable information, and encourage public inputs into policies for contaminated site management, in order to gain public confidence during remediation and regeneration projects.

Trace Elements in Dominant Species of the Fenghe River, China: Their Relations to Environmental Factors.

The distribution of trace elements (TEs) in water, sediment, riparian soil and dominant plants was investigated in the Fenghe River, Northwestern China. The Fenghe River ecosystem was polluted with Cd, Cr, Hg and Pb. There was a high pollution risk in the midstream and downstream regions and the risk level for Cd was much higher than that of the other elements. The average values of bioconcentration coefficient for Cd and Zn were 2.21 and 1.75, respectively, indicating a large accumulation of Cd and Zn in the studied species. With broad ecological amplitudes, L. Levl. et Vant. Trin., and L. had the greatest TE concentrations in aboveground and belowground biomass of the studied species and were potential biomonitors or phytoremediators for the study area. Multivariate techniques including cluster analysis, correlation analysis, principal component analysis, and canonical correspondence analysis were used to analyze the relations between TE concentrations in plants and various environmental factors. The soil element concentration is the main factor determining the accumulation of TEs in plants. The co-release behavior of common pollutants and TEs drove the accumulation of Hg, Cd, and As in the studied plants. Significant enrichment of some elements in the Fenghe River has led to a decline in the biodiversity of plants.

Estimation of GHG Emissions from Water Reclamation Plants in Beijing.

A procedure for estimating Greenhouse gas (GHG) emissions from a wastewater reclamation plant in Beijing was developed based on the process chain model. GHG emissions under two typical water reclamation treatment processes, the coagulation-sedimentation-filtration traditional process and advanced biological treatment process, were examined. The total on-site GHG emissions were estimated to be 0.0056 kg/m3 and 0.6765 kg/m3 respectively, while total off-site GHG emissions were estimated to be 0.3699 kg/m3 and 0.4816 kg/m3. The overall GHG emissions were 0.3755 kg/m3 under the type 1 treatment, which is much lower than that under the type 2 of 1.1581 kg/m3. Emissions from both processes were lower than that from the tap water production. Wastewater reclamation and reuse should be promoted as it not only saves the water resources but also can reduce the GHG emissions. Energy consumption was the most significant source of GHG emissions. Biogas recovery should be employed as it can significantly reduce the GHG emissions, especially under the type 2 treatment process. Considering the wastewater treatment and reclamation process as a whole, the type 2 treatment process has advantages in reducing the GHG emissions per unit of pollutant. This paper provides scientific basis for decision making.

Wastewater reclamation and reuse in China: Opportunities and challenges.

The growing water stress both in terms of water scarcity and quality deterioration promotes the development of reclaimed water as a new water resource use. This paper reviewed wastewater reuse practices in China, and the opportunities and challenges of expanding reclaimed water use were analyzed. Rapid urbanization with the increasing of water demand and wastewater discharge provides an opportunity for wastewater reuse. The vast amount of wastewater discharge and low reclaimed water production mean that wastewater reuse still has a great potential in China. Many environmental and economic benefits and successful reclamation technologies also provide opportunities for wastewater reuse. In addition, the overall strategy in China is also encouraging for wastewater reuse. In the beginning stage of wastewater reclamation and reuse, there are many significant challenges to expand wastewater reuse in China including slow pace in adopting urban wastewater reuse programs, the establishment of integrated water resources management framework and guidelines for wastewater reuse programs, incoherent water quality requirements, the limited commercial development of reclaimed water and the strengthening of public awareness and cooperation among stakeholders.

Distribution and bioaccumulation of lead in the coastal watersheds of the Northern Bohai and Yellow Seas in China.

In this study, the concentration of lead ([Pb]) in the surface water, sediments, soils and muscles of carp and crab in the upstream and downstream coastal watersheds along the Northern Bohai and Yellow Seas (NBYS) in China was investigated and the risks of Pb were evaluated. The mean [Pb] in the downstream water (2.62 µg/L) and sediments [24.5 mg/kg, dry mass (dm)] was greater than the Chinese seawater quality standard for class I (1 µg/L) and the regional background soil concentration (11.5 mg Pb/kg, dm), respectively. Approximately 37 % of the soils, mainly from the upstream regions, had [Pb] greater than the regional background concentration of 21.4 mg/kg, dm. The sites with relatively large [Pb] in the water, sediments and soils were located in the coastal watersheds of Tangshan and Huludao. The large enrichment factors in the sediments (2.41) and soils (2.22) suggested that human activities influenced the soils and sediments in this region more than in the other regions. Relatively large [Pb] was found in the crabs that were obtained from the upstream reaches of the Shuanglong and Daliao Rivers and the downstream reaches of the Luanhe and Liugu Rivers. Most of the crabs from the upstream regions contained greater [Pb] than the permissible limit for human consumption [0.3 mg/kg, wet mass (wm)]. The risk indices of the water, carp and crabs for humans were 0.002, 0.01 and 0.006, respectively. Based on the bioaccumulation factors, biota-sediment accumulation factors (BSAFs) and human risk indices, it was concluded that the human risks associated with crab were lower than those of carp despite the greater accumulation of Pb by the crabs from the water and sediments. Finally, the [Pb] in the sediments was significantly correlated with the [Pb] in the soils, which indicated that the same sources of Pb were responsible for the [Pb] in the sediments and soils in the coastal watersheds of the NBYS in China.