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Halogenated flame retardants in wild, prey-sized mud carp from an e-waste recycling site in South China, 2006–2016: Residue dynamics and ecological risk assessment 全文
2021
Wu, Jiang-Ping | Feng, Wen-Lu | Tao, Lin | Li, Xiao | Nie, You-Tian | Xu, Ya-Chun | Zeng, Yan-Hong | Luo, Xiao-Jun | Mai, Bi-Xian
The crude e-waste recycling has been regulated in China since the late 2000s; however, information on the recent levels and the ecological risks of e-waste derived contaminants such as halogenated flame retardants (HFRs) in the e-waste sites are limited. We therefore examined the concentrations of several HFRs in wild, prey-sized mud carps collected from a typical e-waste site in 2006, 2011 and 2016, to understand the exposure dynamics and ecological risk of these chemicals. Several ecological and biological parameters including δ¹⁵N, δ¹³C, body size and lipid content of the fish were also examined, to ensure an overall uniformity of the sample set among the sampling years. Among the HFRs measured, polybrominated diphenyl ethers (PBDEs) were detected at the highest concentrations (contributing >90% to ∑HFRs), followed by Dechlorane Plus (DPs), polybrominated biphenyls (PBBs), and alternative brominated flame retardants (ABFRs). The fish concentrations of ∑PBDEs, ∑PBBs and ∑DPs significantly dropped by 65%, 57% and 53% from 2006 to 2011, and 12%, 74% and 51% from 2011 to 2016, respectively; likely reflecting the positive impact of the environmental regulations on crude e-waste recycling. The ∑ABFRs concentrations were also decreased by 80% from 2006 to 2011, but increased by 127% from 2011 to 2016; suggesting possible fresh input of these novel HFRs in recent years. In addition to the changes in the HFR concentrations, contaminant profiles in the fish were also changed, possibly due to environmental degradation of the HFRs. Despite our conservative method of risk assessment, we found that PBDEs posed an important risk both for the mud carp and for piscivorous wildlife that inhabit the e-waste site.
显示更多 [+] 显示较少 [-]Improving accuracy of air pollution exposure measurements: Statistical correction of a municipal low-cost airborne particulate matter sensor network 全文
2021
Considine, Ellen M. | Reid, Colleen E. | Ogletree, Michael R. | Dye, Timothy
Low-cost air quality sensors can help increase spatial and temporal resolution of air pollution exposure measurements. These sensors, however, most often produce data of lower accuracy than higher-end instruments. In this study, we investigated linear and random forest models to correct PM₂.₅ measurements from the Denver Department of Public Health and Environment (DDPHE)’s network of low-cost sensors against measurements from co-located U.S. Environmental Protection Agency Federal Equivalence Method (FEM) monitors. Our training set included data from five DDPHE sensors from August 2018 through May 2019. Our testing set included data from two newly deployed DDPHE sensors from September 2019 through mid-December 2019. In addition to PM₂.₅, temperature, and relative humidity from the low-cost sensors, we explored using additional temporal and spatial variables to capture unexplained variability in sensor measurements. We evaluated results using spatial and temporal cross-validation techniques. For the long-term dataset, a random forest model with all time-varying covariates and length of arterial roads within 500 m was the most accurate (testing RMSE = 2.9 μg/m³ and R² = 0.75; leave-one-location-out (LOLO)-validation metrics on the training set: RMSE = 2.2 μg/m³ and R² = 0.93). For on-the-fly correction, we found that a multiple linear regression model using the past eight weeks of low-cost sensor PM₂.₅, temperature, and humidity data plus a near-highway indicator predicted each new week of data best (testing RMSE = 3.1 μg/m³ and R² = 0.78; LOLO-validation metrics on the training set: RMSE = 2.3 μg/m³ and R² = 0.90). The statistical methods detailed here will be used to correct low-cost sensor measurements to better understand PM₂.₅ pollution within the city of Denver. This work can also guide similar implementations in other municipalities by highlighting the improved accuracy from inclusion of variables other than temperature and relative humidity to improve accuracy of low-cost sensor PM₂.₅ data.
显示更多 [+] 显示较少 [-]Enhancing inhibition of disinfection byproducts formation and opportunistic pathogens growth during drinking water distribution by Fe2O3/Coconut shell activated carbon 全文
2021
Xing, Xueci | Li, Tong | Bi, Zhihao | Qi, Peng | Li, Zesong | Wang, Haibo | Lyu, Lai | Gao, Yaowen | Hu, Jun
The effects of biological activated carbon treatment using Fe₂O₃ modified coconut shell-based activated carbon (Fe/CAC) were investigated on the occurrence of opportunistic pathogens (OPs) and formation of disinfection by-products (DBPs) in simulated drinking water distribution systems (DWDSs) with unmodified CAC as a reference. In the effluent of annular reactor (AR) with Fe/CAC, the OPs growth and DBPs formation were inhibited greatly. Based on the differential pulse voltammetry and dehydrogenase activity tests, it was verified that extracellular electron transfer was enhanced in the attached biofilms of Fe/CAC, hence improving the microbial metabolic activity and biological removal of organic matter especially DBPs precursors. Meanwhile, the extracellular polymeric substances (EPS) on the surface of Fe/CAC exhibited stronger viscosity, higher flocculating efficiency and better mechanical stability, avoiding bacteria or small-scale biofilms falling off into the water. Consequently, the microbial biomass and EPS substances amount decreased markedly in the effluent of Fe/CAC filter. More importantly, Fe/CAC did significantly enhance the shaping role on microbial community of downstream DWDSs, continuously excluding OPs advantage and inhibiting EPS production. The weakening of EPS in DWDSs resulted in decrease of microbial chlorine-resistance ability and EPS-derived DBPs precursors supply. Therefore, the deterioration of water quality in DWDSs was inhibited greatly, sustainably maintaining the safety of tap water. Our findings indicated that optimizing biological activated carbon treatment by interface modification is a promising method for improving water quality in DWDSs.
显示更多 [+] 显示较少 [-]Synthesis of oxygen vacancy-enriched N/P co-doped CoFe2O4 for high-efficient degradation of organic pollutant: Mechanistic insight into radical and nonradical evolution 全文
2021
Hu, Mingzhu | Zhu, Jinyi | Zhou, Wenjun
Oxygen vacancy-enriched N/P co-doped cobalt ferrite (NPCFO) was synthesized using ionic liquid as N and P sources, and then the catalytic performance and mechanism of NPCFO upon peroxymonosulfate (PMS) activation for the degradation of organic pollutants were investigated. The as-synthesized NPCFO-700 exhibited excellent catalytic performance in activating PMS, and the degradation rate constant of 4-chlorophenol (4-CP) increased with the increase of OV concentration in NPCFO-x. EPR analysis confirmed the existence of ·OH, SO₄·⁻, and ¹O₂ in the NPCFO-700/PMS system, in which OV could induce the generation of ¹O₂ by PMS adsorption and successive capture, and also served as electronic transfer medium to accelerate the redox cycle of M²⁺/M³⁺ (M denotes Co or Fe) for the generation of radical to synergistically degrade organic pollutants. In addition, the contribution of free radical and nonradical to 4-CP degradation was observed to be strongly dependent on solution pH, and SO₄·⁻ was the major ROS in 4-CP degradation under acid and alkaline condition, while ¹O₂ was involved in the degradation of 4-CP under neutral condition due its selective oxidation capacity, as evidenced by the fact that such organic pollutants with ionization potential (IP) below 9.0 eV were more easily attacked by ¹O₂. The present study provided a novel insight into the development of transition metal-based heterogeneous catalyst containing massive OV for high-efficient PMS activation and degradation of organic pollutants.
显示更多 [+] 显示较少 [-]Characterization and source apportionment of single particles from metalworking activities 全文
2021
Arndt, Jovanna | Healy, Robert M. | Setyan, Ari | Flament, Pascal | Deboudt, Karine | Riffault, Véronique | Alleman, Laurent Y. | Mbengue, Saliou | Wenger, John C.
Industrial metalworking facilities emit a variety of air toxics including volatile organic compounds, polycyclic aromatic hydrocarbons (PAHs) and heavy metals. In order to investigate these emissions, a 1-month multi-instrument field campaign was undertaken at an industrial site in Grande-Synthe, Dunkirk (France), in May and June 2012. One of the main objectives of the study was to provide new information on the chemical composition of particulate matter with aerodynamic diameters smaller than 2.5 μm (PM₂.₅) in the vicinity of metalworking facilities. An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed to provide size-resolved chemical mixing state measurements of ambient single particles at high temporal resolution. This mixing state information was then used to apportion PM₂.₅ to local metalworking facilities influencing the receptor site. Periods when the site was influenced by metalworking sources were characterised by a pronounced increase in particles containing toxic metals (manganese, iron, lead) and polycyclic aromatic hydrocarbons (PAHs) with a variety of chemical mixing states. The association of specific particle classes with a nearby ferromanganese alloy manufacturing plant was confirmed through comparison with previous analysis of raw materials (ores) and chimney filter particle samples collected at the facility. Particles associated with emissions from a nearby steelworks were also identified. The contribution of local metalworking activities to PM₂.₅ at the receptor site for the period when the ATOFMS was deployed ranged from 1 to 65% with an average contribution of 17%, while the remaining mass was attributed to other local and regional sources. These findings demonstrate the impact of metalworking facilities on air quality downwind and provide useful single particle signatures for future source apportionment studies in communities impacted by metalworking emissions.
显示更多 [+] 显示较少 [-]Effects of plant growth regulator and chelating agent on the phytoextraction of heavy metals by Pfaffia glomerata and on the soil microbial community 全文
2021
Huang, Rong | Cui, Xiaoying | Luo, Xianzhen | Mao, Peng | Zhuang, Ping | Li, Yongxing | Li, Yingwen | Li, Zhian
Pfaffia glomerata is a candidate for the remediation of heavy metal-contaminated soil, but phytoremediation efficiency requires enhancement. In this study, we evaluated how application of DA-6, EDTA, or CA affected the growth and heavy metal accumulation of P. glomerata and soil microorganisms. We found that P. glomerata removed more Cd and Zn than Pb or Cu from contaminated soil. When compared to the control, application of DA-6, CA, or CA + DA-6 increased plant biomass and increased stem Cd concentration by 1.28-, 1.20-, and 1.31-fold respectively; increased leaf Cd concentration by 1.25-, 1.28-, and 1.20-fold, respectively; and increased the total quantity of Cd extracted by 1.37-, 1.37-, and 1.38-fold, respectively. When compared to the control, application EDTA or EDTA + DA-6 significantly increased the soil available metal and Na concentrations, which harmed plant growth. Application of EDTA or EDTA + DA-6 also significantly decreased the Cd concentration in roots and stems. 16S rRNA high-throughput sequencing analysis revealed that application of EDTA or CA alone to soil significantly reduced the richness and diversity of soil bacteria, while foliar spraying of DA-6 combined with EDTA or CA slightly alleviated this reduction. EDTA or CA addition significantly changed the proportion of Actinobacteria and Proteobacteria. In addition, EDTA or CA addition caused changes in soil properties (e.g. heavy metal availability, K concentration, Na concentration, soil pH, soil CEC, and soil DOC concentration) that were associated with changes in the bacterial community. EDTA addition mainly affected the soil bacterial community by changing soil DOC concentration, the soil available Pb and Na concentration, and CA addition mainly affected the soil bacterial community by changing the soil available Ca concentration.
显示更多 [+] 显示较少 [-]Long-term variations of C1–C5 alkyl nitrates and their sources in Hong Kong 全文
2021
Zeng, Lewei | Guo, Hai | Lyu, Xiaopu | Zhou, Beining | Ling, Zhenhao | Simpson, Isobel J. | Meinardi, Simone | Barletta, Barbara | Blake, Donald R.
Investigating the long-term trends of alkyl nitrates (RONO₂) is of great importance for evaluating the variations of photochemical pollution. Mixing ratios of C₁–C₅ RONO₂ were measured in autumn Hong Kong from 2002 to 2016, and the average level of 2-butyl nitrate (2-BuONO₂) always ranked first. The C₁–C₄ RONO₂ all showed increasing trends (p < 0.05), and 2-BuONO₂ had the largest increase rate. The enhancement in C₃ RONO₂ was partially related to elevated propane, and dramatic decreases (p < 0.05) in both nitrogen monoxide (NO) and nitrogen dioxide (NO₂) also led to the increased RONO₂ formation. In addition, an increase of hydroxyl (OH) and hydroperoxyl (HO₂) radicals (p < 0.05) suggested enhanced atmospheric oxidative capacity, further resulting in the increases of RONO₂. Source apportionment of C₁–C₄ RONO₂ specified three typical sources of RONO₂, including biomass burning emission, oceanic emission, and secondary formation, of which secondary formation was the largest contributor to ambient RONO₂ levels. Mixing ratios of total RONO₂ from each source were quantified and their temporal variations were investigated. Elevated RONO₂ from secondary formation and biomass burning emission were two likely causes of increased ambient RONO₂. By looking into the spatial distributions of C₁–C₅ RONO₂, regional transport from the Pearl River Delta (PRD) was inferred to build up RONO₂ levels in Hong Kong, especially in the northwestern part. In addition, more serious RONO₂ pollution was found in western PRD region. This study helps build a comprehensive understanding of RONO₂ pollution in Hong Kong and even the entire PRD.
显示更多 [+] 显示较少 [-]O2 distribution and dynamics in the rhizosphere of Phragmites australis, and implications for nutrient removal in sediments 全文
2021
Li, Cai | Ding, Shiming | Ma, Xin | Chen, Musong | Zhong, Zhilin | Zhang, Yi | Ren, Mingyi | Zhang, Min | Yang, Liyuan | Rong, Nan | Wang, Yan
Root-triggered microscale variations in O₂ distribution in the rhizosphere of young Phragmites australis are important for nutrient removal in sediments. In this study, the micro-scale O₂ dynamics and the small-scale changes of soluble reactive phosphorus (SRP) and ammonium (NH₄⁺) in the rhizosphere of P. australis were investigated using planar optodes and high-resolution dialysis (HR-Peeper), respectively. Results suggested that root O₂ leakage has a highly variable distribution depending on the stage of root growth, the site of O₂ leakage gradually shift from the entire emerging main roots to the main root tip and subsequently shifted the emerging lateral roots. The O₂ concentration increased in the rhizosphere with increasing light intensity and O₂ levels in the overlying water. Continuous O₂ release from the lateral roots causes the formation of iron plaque on the surface of lateral roots, which reduce the mobility of P by adsorption of iron plaque in the rhizosphere. The oscillation of oxic-anoxic root zones improves nitrogen removal through the processes of anammox, heterotrophic denitrification and nitrification. This work from the micro-scale demonstrates that the O₂ concentration is the spatio-temporal variations in the rhizosphere, and it presents an important role for nutrient removal in sediments.
显示更多 [+] 显示较少 [-]Random forest model based fine scale spatiotemporal O3 trends in the Beijing-Tianjin-Hebei region in China, 2010 to 2017 全文
2021
Ma, Runmei | Ban, Jie | Wang, Qing | Zhang, Yayi | Yang, Yang | He, Mike Z. | Li, Shenshen | Shi, Wenjiao | Li, Tiantian
Ambient ozone (O₃) concentrations have shown an upward trend in China and its health hazards have also been recognized in recent years. High-resolution exposure data based on statistical models are needed. Our study aimed to build high-performance random forest (RF) models based on training data from 2013 to 2017 in the Beijing-Tianjin-Hebei (BTH) region in China at a 0.01 ° × 0.01 ° resolution, and estimated daily maximum 8h average O₃ (O₃-8hmax) concentration, daily average O₃ (O₃-mean) concentration, and daily maximum 1h O₃ (O₃-1hmax) concentration from 2010 to 2017. Model features included meteorological variables, chemical transport model output variables, geographic variables, and population data. The test-R² of sample-based O₃-8hmax, O₃-mean and O₃-1hmax models were all greater than 0.80, while the R² of site-based and date-based model were 0.68–0.87. From 2010 to 2017, O₃-8hmax, O₃-mean, and O₃-1hmax concentrations in the BTH region increased by 4.18 μg/m³, 0.11 μg/m³, and 4.71 μg/m³, especially in more developed regions. Due to the influence of weather conditions, which showed high contribution to the model, the long-term spatial distribution of O₃ concentrations indicated a similar pattern as altitude, where high concentration levels were distributed in regions with higher altitude.
显示更多 [+] 显示较少 [-]Sustainable stabilization/solidification of the Pb, Zn, and Cd contaminated soil by red mud-derived binders 全文
2021
Wang, Fei | Xu, Jian | Yin, Hailong | Zhang, Yunhui | Pan, Hao | Wang, Lei
Red mud and phosphogypsum are voluminous industrial by-products worldwide. They have long been disposed of in landfills or open storage, leading to a waste of resource and environmental pollution. This study provides a novel approach to recycle these industrial by-products as sustainable red mud-phosphogypsum-Portland cement (RPPC) binders for stabilization/solidification (S/S) of multimetal-contaminated soil. The physical strength, metal leachability and microstructure of S/S soil were investigated after 7-day and 28-day curing, as well as freezing-thawing (F-T) cycle and wetting-drying (W-D) cycle. The results show that the strength of soil treated by all binders fulfilled the uniaxial compressive strength requirement (350 kPa) of S/S waste in landfills. Microstructural analyses show that the main hydration products of the RPPC S/S soil are ilmenite, ettringite, anhydrite and hydrated calcium silicate. The 10% and 15% RPPC binders have a competitive metal immobilization ability compared with 10% PC, but the immobilization priority is different: Pb > Zn > Cd in RPPC system and Zn > Cd > Pb in PC system, respectively, probably due to the precipiataion of Pb²⁺ with the abundant SO₄²⁻ in phosphogypsum in RPPC system. The strength of RPPC and PC treated soil was still higher than 350 kPa except for RPPC7.5 after 10 freeze-thaw or 10 wetting-drying cycles. The RPPC binder performed worse than PC binder after both freeze-thaw and wetting-drying cycles, especially at a lower dosage. Only the metal leaching concentrations of samples treated by RPPC15 and PC10 could fulfil the Chinese standards for hazardous wastes.
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