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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.
Show more [+] Less [-]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.
Show more [+] Less [-]Association of exposures to perchlorate, nitrate, and thiocyanate with allergic symptoms: A population-based nationwide cohort study
2021
Zhu, Fanghuan | Jiao, Jingjing | Zhuang, Pan | Huang, Mengmeng | Zhang, Yu
Allergic diseases have been one of the leading causes of chronic disorders in the United States. Animal studies have suggested that exposures to perchlorate, nitrate, and thiocyanate could induce allergic inflammation. However, the associations have not been examined among general populations. Here, we investigated data of 7030 participants aged ≥6 years from the National Health and Nutritional Examination Survey (NHANES) 2005–2006. Urinary levels of perchlorate, nitrate, and thiocyanate were measured by ion chromatography combined with electrospray tandem mass spectrometry. Information on allergic symptoms (hay fever, allergy, rash, sneeze, wheeze, eczema, and current asthma) was collected by questionnaire. Allergic sensitization was defined by a concentration ≥150 kU/L for total immunoglobulin E (IgE) levels. The associations were estimated using multivariate-adjusted logistic regression models. A positive association was observed for urinary nitrate and eczema (p < 0.001 for the trend). Compared with quartile 1 (lowest quartile), the odds ratios of eczema with 95% confidence intervals [ORs (95% CIs)] from quartiles 2 to 4 were 1.72 (95% CI, 1.41, 2.09), 1.94 (1.53, 2.47) and 2.10 (1.49, 2.97) for urinary nitrate. In addition, urinary thiocyanate was positively related to sneeze (ORQ₄ ᵥₛ. Q₁: 1.25, 95% CI: 1.01, 1.55; p = 0.015 for the trend). However, urinary perchlorate was not correlated with any allergic-related outcome. Additionally, the associations were different among subgroups in a four-level polytomous model. Thus, our results suggested that exposures to nitrate and thiocyanate may be associated with allergic symptoms. Further investigations are warranted to concentrate on the practical strategies to monitor exposure levels and the latent mechanisms of the relationship between exposure and allergy.
Show more [+] Less [-]Evolution of secondary inorganic aerosols amidst improving PM2.5 air quality in the North China plain
2021
Zhang, Yangyang | Liu, Xuejun | Zhang, Lin | Tang, Aohan | Goulding, K. W. T. | Collett, Jeffrey L.
The Clean Air Action implemented by the Chinese government in 2013 has greatly improved air quality in the North China Plain (NCP). In this work, we report changes in the chemical components of atmospheric fine particulate matter (PM₂.₅) at four NCP sampling sites from 2012/2013 to 2017 to investigate the impacts and drivers of the Clean Air Action on aerosol chemistry, especially for secondary inorganic aerosols (SIA). During the observation period, the concentrations of PM₂.₅ and its chemical components (especially SIA, organic carbon (OC), and elemental carbon (EC)) and the frequency of polluted days (daily PM₂.₅ concentration ≥ 75 μg m⁻³) in the NCP, declined significantly at all four sites. Asynchronized reduction in SIA components (large decreases in SO₄²⁻ with stable or even increased NO₃⁻ and NH₄⁺) was observed in urban Beijing, revealing a shift of the primary form of SIA, which suggested the fractions of NO₃⁻ increased more rapidly than SO₄²⁻ during PM₂.₅ pollution episodes, especially in 2016 and 2017. In addition, unexpected increases in the sulfur oxidation ratio (SOR) and the nitrogen oxidation ratio (NOR) were observed among sites and across years in the substantially decreased PM₂.₅ levels. They were largely determined by secondary aerosol precursors (i.e. decreased SO₂ and NO₂), photochemical oxidants (e.g. increased O₃), temperature, and relative humidity via gas-phase and heterogeneous reactions. Our results not only highlight the effectiveness of the Action Plan for improving air quality in the NCP, but also suggest an increasing importance of SIA in determining PM₂.₅ concentration and composition.
Show more [+] Less [-]Mitigating NOX emissions does not help alleviate wintertime particulate pollution in Beijing-Tianjin-Hebei, China
2021
Li, Xia | Bei, Naifang | Hu, Bo | Wu, Jiarui | Pan, Yuepeng | Wen, Tianxue | Liu, Zirui | Liu, Lang | Wang, Ruonan | Li, Guohui
Stringent mitigation measures have reduced wintertime fine particulate matter (PM₂.₅) concentrations by 42.2% from 2013 to 2018 in the Beijing-Tianjin-Hebei (BTH) region, but severe PM pollution still frequently engulfs the region. The observed nitrate aerosols have not exhibited a significant decreasing trend and constituted a major fraction (about 20%) of the total PM₂.₅, although the surface-measured NO₂ concentration has decreased by over 20%. The contributions of nitrogen oxides (NOX) emissions mitigation to the nitrate and PM₂.₅ concentrations and how to alleviate nitrate aerosols efficiently under the current situation still remains elusive. The WRF-Chem model simulations of a persistent and heavy PM pollution episode in January 2019 in the BTH reveal that NOX emissions mitigation does not help lower wintertime nitrate and PM₂.₅ concentrations under current conditions in the BTH. A 50% reduction in NOX emissions only decreases nitrate mass by 10.3% but increases PM₂.₅ concentrations by 3.2%, because the substantial O₃ increase induced by NOX mitigation offsets the HNO₃ loss and enhances sulfate and secondary organic aerosols formation. Our results are further consolidated by the occurrence of severe PM pollution in the BTH during the COVID-19 outbreak, with a significant reduction in NO₂ concentration. Mitigation of NH₃ emissions constitutes the priority measure to effectively lower the nitrate and PM₂.₅ concentrations in the BTH under current conditions, with 35.5% and 12.7% decrease, respectively, when NH₃ emissions are reduced by 50%.
Show more [+] Less [-]Wintertime chemical characteristics of aerosol and their role in light extinction during clear and polluted days in rural Indo Gangetic plain
2021
Izhar, Saifi | Gupta, Tarun | Qadri, Adnan Mateen | Panday, Arnico K.
This paper reports the chemical and light extinction characteristics of fine aerosol (PM₂.₅) during the winter period (2017–18) at Lumbini, Nepal, a rural site on the Indo Gangetic Plains. A modified IMPROVE algorithm was employed to reconstruct light extinction by chemical constituents of aerosol. The fine aerosol levels impacted visibility adversely during daytime, but during nighttime visibility was controlled by fog droplets rather than by aerosols. The PM₂.₅ chemical constituents showed varying characteristics during clear and polluted days. The average NO₃⁻/SO₄²⁻ concentration ratio was 0.57 during clear and 1.36 and polluted days, signifying a change in secondary inorganics and formation processes mainly due to decreasing photochemical production and due to increased partitioning of nitrate particles at a lower temperature. The increased secondary organics contribution and the higher OM/OC ratio (2.2) during polluted days showed the vital role of aqueous processing and biomass burning emissions in determining the concentration of organics. Total light extinction was 2.3 times higher on polluted days compared to clear days, while the PM₂.₅ mass concentration was 1.5 times higher. This variation in mass and extinction order signifies that various chemical components in fine particles have a more considerable impact on light extinction. On clear days we found that carbonaceous particles (OM and EC) made a major contribution to light extinction. In contrast, the extinction contribution by secondary inorganic (especially NH₄NO₃) increased significantly during polluted days, with hygroscopic growth and enhanced scattering efficiency at higher RH conditions playing a major role. The comparison between clear and polluted days altogether suggests that regulating the nitrate sources can help significantly in improving the visibility levels and restrict fog haze development during wintertime in rural IGP.
Show more [+] Less [-]Contrasting sources and fate of nitrogen compounds in different groundwater systems in the Central Yangtze River Basin
2021
Xiong, Yaojin | Du, Yao | Deng, Yamin | Ma, Teng | Li, Dian | Sun, Xiaoliang | Liu, Guangning | Wang, Yanxin
Although groundwater nitrogen pollution has been widely studied, the control of hydrogeological conditions on behavior of nitrogen compounds has been poorly understood. In this study, multiple stable isotopes (N/C/H/O), spectral characteristics of DOM coupled with water chemistry were used to reveal the sources and fate of nitrate and ammonium in three subareas with different hydrogeological conditions in the Central Yangtze River Basin. We identified three contrasting patterns of nitrogen sources and fate in groundwater controlled by different aquifer features. In a reducing porous aquifer mainly composed of carbonate minerals overlain by a thick low-permeability layer, the NH₄–N concentration is high (mean 4.12 mg/L) but with quite low NO₃–N concentration (mean 0.28 mg/L). The high ammonium is mainly from intense degradation of organic matter (OM), while denitrification at a higher rate results in nitrate removal. Feammox may be favored owing to abundant humics acting as the electron shuttle. In a weakly reducing to oxidizing porous aquifer mainly composed of aluminosilicate minerals overlain by a varying thickness of low-permeability layer, high ammonium occurs in a weakly reducing condition and is affected by both anthropogenic input and OM degradation, while high nitrate occurs in a more oxidizing condition and could be mainly from soil nitrogen, manure or sewage. Feammox may be also favored due to more acidic environment formed by weathering of aluminosilicate minerals, fluctuating redox condition and low abundance of labile organic carbon, while denitrification occurs at a slower rate coupled with concurrent re-oxidation of nitrite to nitrate. In an oxidizing porous - fissured aquifer system overlain by a thin low-permeability layer, the concentrations of ammonium and nitrate are both low, possibly due to strong hydrodynamic and flushing condition, although slightly higher concentration of nitrate exhibit similar sources and fate with the weakly reducing to oxidizing porous aquifer mentioned above.
Show more [+] Less [-]Current challenges of improving visibility due to increasing nitrate fraction in PM2.5 during the haze days in Beijing, China
2021
Hu, Shuya | Zhao, Gang | Tan, Tianyi | Li, Chengcai | Zong, Taomou | Xu, Nan | Zhu, Wenfei | Hu, Min
The annual mean PM₂.₅ mass concentration has decreased because of the stringent emission controls implemented in Beijing, China in recent years, whereas the nitrate NO3– mass fraction in PM₂.₅ increases gradually. Low-visibility events occur frequently even though PM₂.₅ pollution has been mitigated significantly, with the daily mean PM₂.₅ mass concentration mostly less than 75 μg/m³. In this study, the non-linear relationship was analyzed between atmospheric visibility and PM₂.₅ based on chemical composition from a two-year field observation. Our results showed that NO3– became the main constituent of PM₂.₅, especially during the haze pollution episodes. A localized parameterization scheme was proposed between the atmospheric extinction coefficient (σext) and major chemical constituents of PM₂.₅ by multiple linear regression (MLR). The contribution of NO3– to σext increased with increasing air pollution, and NO3– became the most important contributor for PM₂.₅ above 75 μg/m³. The visibility decreased with increasing NO3– mass fraction for the same PM₂.₅ mass concentration when PM₂.₅ was above 20 μg/m³. The hygroscopicity of PM₂.₅ increased with increasing mass fraction of hygroscopic NO3–. These results stressed the importance of reducing particulate NO3– and its precursors (for instance, NH₃) through effective emission control measures as well as the tightening of PM₂.₅ standards to further improve air quality and visibility in Beijing.
Show more [+] Less [-]Assessment of the water quality of groundwater in Bohai Rim and the controlling factors—a case study of northern Shandong Peninsula, north China
2021
Gao, Zongjun | Han, Cong | Xu, Yuan | Zhao, Zhenhua | Luo, Zhenjiang | Liu, Jiutan
This study collected 184 groundwater (GW) samples from 92 wells during the dry and wet seasons, respectively to understand the hydrochemical characteristics, water quality, and risk of GW nitrate (NO₃⁻) to human health in northern Shandong Peninsula (NSP), China. The results showed that GW in the NSP is weakly alkaline and classified as hard fresh water. The mean concentration of NO₃⁻ in GW exceeded 100 mg·L⁻¹, total hardness exceeded 450 mg·L⁻¹, and total dissolved solids (TDS) was less than 1000 mg·L⁻¹. A Piper diagram showed that the water chemistry of GW in the NSP was mainly of the SO₄·Cl-Ca·Mg type. A Gibbs diagram and ion ratio analysis indicated that the weathering of silicate rocks and agricultural production were the dominant factors affecting the hydrochemical characteristics of GW in the NSP, with cation exchange, dissolution of salt rock, and weathering of carbonate rock also making contributions. Na⁺ and Cl⁻ in GW are significantly affected by seawater aerosols in coastal areas. During the wet season, the hydrodynamic conditions of the aquifer are improved, agricultural activities are strengthened, and GW becomes generally homogenized. The water quality index classified the GW quality of the NSP as mainly of medium quality. There was a relatively consistent spatial distribution of water quality during different periods. Water samples of poor water quality were mainly distributed in the lower reaches of the Huangshui River. In addition, total hardness and NO₃⁻ concentrations were the main variables affecting the quality of GW in the NSP. The assessment of the risk NO₃⁻ in GW in the NSP to human health through the ingestion of drinking water demonstrated a significant risk (infants > children > adults). These results indicate the need for local management measures to reduce the potential health risks of GW quality in the NSP.
Show more [+] Less [-]Photolysis of polycyclic aromatic hydrocarbons adsorbed on polyethylene microplastics
2021
Noro, Kazushi | Yabuki, Yoshinori
Contaminants adsorbed on microplastics (MPs) are a potential risk to aquatic environments. Several studies have demonstrated that polycyclic aromatic hydrocarbons (PAHs), which adsorb on MPs, can be photolyzed in aqueous solutions. We investigated photolysis of PAHs on MPs under sunlight conditions to estimate their environmental fate for the first time. The PAHs (25 ng each) were added to polyethylene powder, which was used as the MP sample. The MP sample was agitated in water with sunlight irradiation; thereafter, the concentration of the PAHs on the MP sample was determined by high-pressure liquid chromatography with a fluorescence detector. The half-life values of the PAHs were estimated between 3.4 × 10² (pyrene) and 3.2 × 10⁴ min (benz[j]fluoranthene). These values are 0.5 (fluoranthene) to 25 (benzo[a]pyrene) times larger than those in the aqueous phase. Additionally, the degradation of PAHs by OH radicals produced by the photolysis of nitrate was observed.
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