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Transport process and source contribution of nitrogen in stormwater runoff from urban catchments
2021
Ma, Yukun | Wang, Shihui | Zhang, Xiaoyue | Shen, Zhenyao
Nitrogen in urban stormwater has been widely studied, and effective management of nitrogen pollution is critical for improving urban stormwater and receiving water quality. This requires an in-depth understanding of the transport process and source contribution to both dissolved and particulate nitrogen in stormwater from urban catchments. In this study, 123 stormwater runoff samples were collected from an urban catchment during different rainfall events. Dissolved and particulate nitrogen concentrations in roof runoff, road runoff, and sewer flow were analyzed. The concentration of dissolved nitrogen was higher in roof runoff than in road runoff and sewer flow. However, the concentration of particulate nitrogen was lower in roof runoff than in road runoff and sewer flow. Isotopic analysis and Bayesian mixing models showed that road runoff was the largest source contributor of both nitrate and particulate organic nitrogen (PON) in sewer flow discharged from the study catchment. In addition, road runoff contributed the majority of PON associated with coarse particles (>105 μm), whereas PON associated with fine particles (<105 μm) was primarily washed-off of sewer sediments. The results provided several suggestions for the management of nitrogen pollution in urban catchments. This study could help to fully understand the transport and sources of nitrogen pollution in urban stormwater and provide recommendations to the government for implementing appropriate stormwater management strategies to minimize stormwater pollution.
显示更多 [+] 显示较少 [-]Iron turning waste: Low cost and sustainable permeable reactive barrier media for remediating dieldrin, endrin, DDT and lindane in groundwater
2021
Abbas, Tauqeer | Wadhawan, Tanush | Khan, Asad | McEvoy, John | Khan, Eakalak
The feasibility and effectiveness of iron turning waste as low cost and sustainable permeable reactive barrier (PRB) media for remediating dieldrin, endrin, dichlorodiphenyltrichloroethane (DDT), and lindane individually (batch system) and combined (continuous flow column) in water were investigated. After 10 min of reaction in a batch system, removal of endrin, dieldrin, and DDT was higher (86–91 %) than lindane (41 %) using 1 g of iron turning waste in 200 mL of pesticide solution (20 μg/L for each pesticide). Among the studied pesticides, only lindane removal decreased substantially in the presence of nitrate (37 %) and magnesium (18 %). Acidic water environment (pH = 4) favored the pesticide removal than neutral and basic environments. For the column experiments, sand alone as PRB media was ineffective for remediating the pesticides in water. When only iron turning was used, the removal efficiencies of lindane, endrin, and dieldrin were 83–88 % and remained stable during 60 min of the experiments. DDT removal was less than other pesticides (58 %). Sandwiching the iron turning waste media between two sand layers improved DDT removal (79 %) as well as limited the iron content below a permissible level in product water. In a long-term PRB column performance evaluation, iron turning waste (150 g) removed all pesticides in water (initial concentration of each pesticide = 2 μg/L) effectively (≥94 %) at a hydraulic retention time of 1.6 h. Iron turning waste, which was mainly in the form of zerovalent iron (Fe⁰), was oxidized to ferrous (Fe²⁺) and ferric (Fe³⁺) iron during its reaction with pesticides, and electrons donated by Fe⁰ and Fe²⁺ were responsible for complete dechlorination of all the pesticides. Therefore, it can be used as inexpensive and sustainable PRB media for groundwater remediation especially in developing countries where groundwater contamination with pesticides is more prevalent.
显示更多 [+] 显示较少 [-]Characterization of the hydrochemistry of water resources of the Weibei Plain, Northern China, as well as an assessment of the risk of high groundwater nitrate levels to human health
2021
Liu, Jiutan | Peng, Yuming | Li, Changsuo | Gao, Zongjun | Chen, Shaojie
This study aimed to evaluate the hydrochemistry of the water resources of the Weibei Plain, Northern China, as well as the risks posed by high groundwater nitrate concentrations to human health. Groundwater and surface water samples numbering 168 and 14, respectively, were collected during the dry and wet seasons. Water in the study area was weakly alkaline, falling into a hard-fresh or hard-brackish category. The groundwater chemical types were mainly SO₄·Cl–Ca·Mg (59.5%) and HCO₃–Ca·Mg (28.6%), whereas the dominant chemistry type of surface water was SO₄·Cl–Na (78.6%). Groundwater showed relatively high concentrations of NO₃⁻, with average dry and wet season concentrations of 212 mg·L⁻¹ and 223 mg·L⁻¹, respectively, whereas surface water had a low NO₃⁻ content. The major processes affecting water chemistry were determined to be rock weathering, such as silicate weathering and evaporative dissolution, as well as cation exchange. NO₃⁻ in groundwater was found to mainly originate from anthropogenic inputs such as agricultural production and domestic sewage. The entropy-weight water quality index (EWQI) assessment showed that although the quality of surface water was generally good, more than half of the groundwater samples failed drinking water standards, with NO₃⁻ identified as being the most problematic parameter affecting the water quality evaluation. Risk assessment of high groundwater nitrate concentrations indicated that long-term domestic use of groundwater in the study area can put the health of residents at great risk. Totals of 81% and 75% of the groundwater samples exceeded the acceptable limit for non-carcinogenic risk (HI = 1) to infants during the dry and wet seasons, respectively, whereas 75% and 71.3% of samples exceeded the acceptable limit for children, respectively. Future management of water in the Weibei Plain should prioritize the control groundwater nitrate pollution.
显示更多 [+] 显示较少 [-]Source apportionment of marine atmospheric aerosols in northern South China Sea during summertime 2018
2021
Liang, Baoling | Cai, Mingfu | Sun, Qibin | Zhou, Shengzhen | Zhao, Jun
Marine atmospheric aerosols play important roles in the global radiation balance and climate change. Hence, measuring physiochemical aerosol properties is essential to better understand their formation, aging processes, and source origins. However, high temporal resolution measurements of submicron particles are currently scarce in the northern South China Sea (SCS). In this study, we conducted a ship-based cruise campaign with a scanning mobility particle sizer and an online time of flight aerosol chemical speciation monitor to measure the particle number size distribution (PNSD) and the chemical composition of submicron particles over the northern SCS during summer 2018. The mean concentration of non-refractory submicron particulate matter (NR-PM₁) was generally 9.11 ± 4.86 μg m⁻³; sulfate was the most abundant component, followed by organics, ammonium, nitrate, and chloride. Positive matrix factorization (PMF) analysis was applied to the PNSD (size PMF) and organic aerosols (OA PMF) and further investigated the source apportionment of the submicron particles. The size PMF identified four factors, including ship exhaust, ship influencing marine primary, continent affected marine secondary, and mixed accumulation aerosols. The most abundant particles in the number concentration were associated with ship emissions, which accounted for approximately 44 %. The submicron organic aerosols were highly oxidized and composed of low-volatility oxygenated OA (LV-OOA, 68 %), semi-volatile OOA (SV-OOA, 21 %), and hydrocarbon-like OA (HOA, 11 %). The backward trajectory of air masses showed that the northern SCS was most frequently (64.7 %) influenced by air masses from the Indo-Chinese Peninsula (ICP) during the campaign, implying that pollutants from ICP have a significant impact on the atmosphere of the northern SCS during summer. Thus, in situ ship-based cruise measurements can provide valuable data on the physiochemical characteristics of marine atmospheric aerosols to better understand their source origins.
显示更多 [+] 显示较少 [-]Oxidation and sources of atmospheric NOx during winter in Beijing based on δ18O-δ15N space of particulate nitrate
2021
Zhang, Zhongyi | Guan, Hui | Xiao, Hongwei | Liang, Yue | Zheng, Nengjian | Luo, Li | Liu, Cheng | Fang, Xiaozhen | Xiao, Huayun
The determination of both stable nitrogen (δ¹⁵N–NO₃⁻) and stable oxygen (δ¹⁸O–NO₃⁻) isotopic signatures of nitrate in PM₂.₅ has shown potential for an approach of assessing the sources and oxidation pathways of atmospheric NOx (NO+NO₂). In the present study, daily PM₂.₅ samples were collected in the megacity of Beijing, China during the winter of 2017–2018, and this new approach was used to reveal the origin and oxidation pathways of atmospheric NOx. Specifically, the potential of field δ¹⁵N–NO₃⁻ signatures for determining the NOx oxidation chemistry was explored. Positive correlations between δ¹⁸O–NO₃⁻ and δ¹⁵N–NO₃⁻ were observed (with R² between 0.51 and 0.66, p < 0.01), and the underlying environmental significance was discussed. The results showed that the pathway-specific contributions to NO₃⁻ formation were approximately 45.3% from the OH pathway, 46.5% from N₂O₅ hydrolysis, and 8.2% from the NO₃+HC channel based on the δ¹⁸O-δ¹⁵N space of NO₃⁻. The overall nitrogen isotopic fractionation factor (εN) from NOx to NO₃⁻ on a daily scale, under winter conditions, was approximately +16.1‰±1.8‰ (consistent with previous reports). Two independent approaches were used to simulate the daily and monthly ambient NOx mixtures (δ¹⁵N-NOx), respectively. Results indicated that the monthly mean values of δ¹⁵N-NOx compared well based on the two approaches, with values of −5.5‰ ± 2.6‰, −2.7‰ ± 1.9‰, and −3.2‰ ± 2.2‰ for November, December, and January (2017–2018), respectively. The uncertainty was in the order of 5%, 5‰ and 5.2‰ for the pathway-specific contributions, the εN, and δ¹⁵N-NOx, respectively. Results also indicated that vehicular exhaust was the key contributor to the wintertime atmospheric NOx in Beijing (2017–2018). Our advanced isotopic perspective will support the future assessment of the origin and oxidation of urban atmospheric NOx.
显示更多 [+] 显示较少 [-]Aerosol water content enhancement leads to changes in the major formation mechanisms of nitrate and secondary organic aerosols in winter over the North China Plain
2021
Chen, Chunrong | Zhang, Haixu | Yan, Weijia | Wu, Nana | Zhang, Qiang | He, Kebin
In recent years, severe air pollution still frequently occurs in winter despite the effective implementation of clean air actions in China. Therefore, field measurements of particle composition and gas precursors were collected from December 1, 2018 to January 15, 2019 at an urban site in a central Chinese city to investigate the existing mechanisms of pollution. The hourly averaged PM₂.₅ concentration during the campaign was 92.7 μg m⁻³, with nitrate and organic aerosol (OA) demonstrated as the principal components. Generally, NO₂ oxidation in the daytime was observed as the major mechanism for nitrate generation, and aerosol water content (AWC) showed its influential role with the associated increases in the nitrogen oxidation and nitrate partitioning ratios. When AWC increased from dozens to hundreds of μg m⁻³ after the afternoon, nocturnal N₂O₅ hydrolysis was demonstrated as the overriding mechanism and provoked extreme contamination of nitrates. Five sources of organic aerosols (OAs) were identified: hydrocarbon-like OAs (HOAs, 16.5%), coal combustion OAs (CCOAs, 19.2%), biomass burning OAs (BBOAs, 9.9%), semi-volatile oxygenated OAs (SV–OOAs, 29.4%), and low-volatile oxygenated OAs (LV-OOAs, 25.0%). SV-OOAs and LV-OOAs were identified as gasSOAs and aqSOAs according to their sensitivities to the atmospheric oxidation capacity and AWC. In addition, aqueous-phase processing was found to be the dominant pathway for SOA formation when the AWC concentration was higher than 80 μg m⁻³. As an influential factor for nitrate and SOA formation, AWC could be greatly affected by RH and the concentrations of inorganic species. Sulfate, which was mainly contributed by anthropogenic emissions, was demonstrated to be a significant factor for active aqueous phase reactions, although SO₂ has been dramatically reduced in recent years. Above all, this study revealed the significant role of AWC in current pollution episode in winter, and will assist in establishing future measures for pollution mitigation.
显示更多 [+] 显示较少 [-]Influence of modified biochar supported Fe–Cu/polyvinylpyrrolidone on nitrate removal and high selectivity towards nitrogen in constructed wetlands
2021
Hou, Weihao | Wang, Sen | Li, Yue | Hao, Ziran | Zhang, Yi | Kong, Fanlong
In this study, the biochar (BC) supported Fe–Cu bimetallic stabilized by PVP (Fe–Cu/PVP/BC) were prepared and utilized to enhance the nitrate (NO₃⁻) removal and the selectivity toward nitrogen (N₂). Results showed the optimum Fe:Cu:BC ratio and the dosage of the BC (pyrolysis at 700 °C) supported Fe–Cu bimetallic stabilized by polyvinylpyrrolidone (PVP) (Fe–Cu/PVP/BC₇₀₀) were respectively 1:2:3 and 1 mg L⁻¹ with the selectivity toward N₂ of 31 %. This was mainly due to the synergy among Fe⁰, Cu⁰ and BC in the Fe–Cu/PVP/BC. The addition of Fe⁰ could reduce the NO₃⁻ through providing electron. The Cu⁰ and BC improved the selectivity of NO₃⁻ to N₂ through forming [Cu–NO₂⁻ₐdₛ] and adjusting redox potential. The addition of Fe–Cu/PVP/BC could supply electrons for denitrification and enhance the relative abundances of Azospira and Thauera related to denitrification to improve NO₃⁻ removal. This result was further confirmed by the variations of denitrifying functional genes (narG, nirK, nirS and nosZ). This research provided an effective method to improve NO₃⁻ removal during surface water treatment in constructed wetlands (CWs) by adding Fe–Cu/PVP/BC.
显示更多 [+] 显示较少 [-]Influence of Tubificidae Limnodrilus and electron acceptors on the environmental fate of BDE-47 in sediments by (14)C-labelling
2021
Liu, Yanhua | Li, Jinrong | Guo, Ruixin | Ji, Rong | Chen, Jianqiu
2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) was difficult to degrade in sediments. In this study, the environmental behavior of BDE-47 with/without the effect of benthos (Tubificidae Limnodrilus) and electron acceptors in sediments was investigated using C-14 tracer. Generally, extractable residues of BDE-47 were dominant in sediment and posed high environment risk. The amount of non-extractable residues (NERs) accounted for 39.0% of initial radioactivity in oxic sediments was significantly higher than those in anoxic sediments (17.6%). Most of NERs were localized in the humin fraction and presented as sequestrated forms. Under oxic conditions, the present of Limnodrilus significantly increased the proportion of NERs in sediment. Limnodrilus accumulated 34.2% of initial radioactivity. Under anoxic conditions, the addition of iron (Ⅲ) [Fe(III)], sulfate and nitrate reduced the environmental risk of BDE-47 with the increase of NERs formation, while manganese (IV) [Mn(IV)] addition had no effect on the formation of NERs. The present of Limnodrilus and electron acceptors promoted the production of metabolites. Meanwhile, BDE-47 changed the microbial community structure of sediments. These findings indicated that the environmental behavior and risk of BDE-47 was affected by benthos and electron acceptors, and the high proportion of sequestrated NERs posed high bioactivity and toxic threat to ecological environment.
显示更多 [+] 显示较少 [-]Size−resolved source apportionment of particulate matter from a megacity in northern China based on one-year measurement of inorganic and organic components
2021
Tian, Yingze | Harrison, Roy M. | Feng, Yinchang | Shi, Zongbo | Liang, Yongli | Li, Yixuan | Xue, Qianqian | Xu, Jingsha
This research apportioned size-resolved particulate matter (PM) contributions in a megacity in northern China based on a full year of measurements of both inorganic and organic markers. Ions, elements, carbon fractions, n-alkanes, polycyclic aromatic hydrocarbons (PAHs), hopanes and steranes in 9 p.m. size fractions were analyzed. High molecular weight PAHs concentrated in fine PM, while most other organic compounds showed two peaks. Both two-way and three-way receptor models were used for source apportionment of PM in different size ranges. The three-way receptor model gave a clearer separation of factors than the two-way model, because it uses a combination of chemical composition and size distributions, so that factors with similar composition but distinct size distributions (like more mature and less mature coal combustion) can be resolved. The three-way model resolved six primary and three secondary factors. Gasoline vehicles and coal and biomass combustion, nitrate and high relative humidity related secondary aerosol, and resuspended dust and diesel vehicles (exhaust and non-exhaust) are the top two contributors to pseudo-ultrafine (<0.43 μm), fine (0.43–2.1 μm) and coarse mode (>2.1 μm) PM, respectively. Mass concentration of PM from coal and biomass combustion, industrial emissions, and diesel vehicle sources showed a bimodal size distribution, but gasoline vehicles and resuspended dust exhibited a peak in the fine and coarse mode, separately. Mass concentration of sulphate, nitrate and secondary organic aerosol exhibited a bimodal distribution and were correlated with temperature, indicating strong photochemical processing and repartitioning. High relative humidity related secondary aerosol was strongly associated with size shifts of PM, NO₃⁻ and SO₄²⁻ from the usual 0.43–0.65 μm to 1.1–2.1 μm. Our results demonstrated the dominance of primary combustion sources in the <0.43 μm particle mass, in contrast to that of secondary aerosol in fine particle mass, and dust in coarse particle mass in the Northern China megacity.
显示更多 [+] 显示较少 [-]Atmospheric ammonia and its effect on PM2.5 pollution in urban Chengdu, Sichuan Basin, China
2021
Huang, Xiaojuan | Zhang, Junke | Zhang, Wei | Tang, Guiqian | Wang, Yuesi
Controlling ammonia (NH₃) emissions has been proposed as a strategy to mitigate haze pollution. To explore the role of NH₃ in haze pollution in Sichuan Basin, where agricultural activities are intense, hourly in situ data of NH₃, as well as nitric acid and secondary inorganic aerosols (SIAs) were gathered in Chengdu from April 2017 to March 2018. We found that NH₃ had an annual mean concentration of 9.7 ± 3.5 (mean ± standard deviation) μg m⁻³, and exhibited seasonal variations (spring > summer > autumn and winter) due to changes in emission sources and meteorological conditions (particularly temperature). Chengdu's atmosphere is generally NH₃-sufficient, especially in the warm seasons, implying that the formation of SIAs is more sensitive to the availability of nitric acid. However, an NH₃ “sufficient-to-deficient” transition was found to occur during winter pollution periods, and the frequency of NH₃ deficiency increased with the aggravation of pollution. Under NH₃-deficient conditions, the nitrogen oxidation ratio increased linearly with the increase in free NH₃, implying that NH₃ contributes appreciably to the formation of nitrate and thus to high PM₂.₅ loadings. No relationships of NH₃ with fossil fuel combustion–related pollutants were found. The NH₃ emissions from farmland and livestock waste in the suburbs of Chengdu and regional transport from west of Chengdu probably contribute to the occurrence of high PM₂.₅ loading in winter and spring, respectively. These results suggest that to achieve effective mitigation of PM₂.₅ in Chengdu, local and regional emission control of NH₃ and NOx synergistically would be effective.
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