ABSTRACT
Aminophenyl sulfone compounds (ASCs) are widely used in various fields, such as the pharmaceutical and textile industries. ASCs and their primary acetylation products are inevitably discharged into the environment. However, the high toxicity of ASCs could be released from the deacetylation of acetylation products. Still, the occurrence and ecological risks of ASCs and their acetylation products remain largely unknown. Here, we integrated all of the existing ASCs based on the core structure, together with their potential acetylation products, to establish a database covering 1105 compounds. By combining the database with R programming, 45 ASCs, sulfonamides, and their acetylation products were identified in the influent and effluent of 19 municipal wastewater treatment plants in 4 cities of China. 13 of them were detected for the first time in the aquatic environment, and 12 acetylation products were newly identified. The cumulative concentrations of 45 compounds in the influent and effluent were in the range of 231-9.96 × 103 and 26-2.70 × 103 ng/L, respectively. The proportion of the unrecognized compounds accounted for 60.6% of the influent and 62.8% of the effluent. Furthermore, nearly half of the ASCs (46.7%), other sulfonamides (49.9%), and their acetylation products (46.2%) were discharged from the effluent, posing a low-to-medium risk to aquatic organisms. The results provide a guideline for future monitoring programs, particularly for sulfadiazine and dronedarone, and emphasize that the ecological risk of ASCs, sulfonamides, and their acetylation products needs to be considered in the aquatic environment.
Subject(s)
Sulfonamides , Wastewater , Water Pollutants, Chemical , Wastewater/chemistry , Sulfonamides/analysis , Acetylation , Anti-Bacterial Agents , Waste Disposal, Fluid , China , Sulfones , Environmental MonitoringABSTRACT
Microbial communities that reduce nitrous oxide (N2O) are divided into two clades, nosZI and nosZII. These clades significantly differ in their ecological niches and their implications for N2O emissions in terrestrial environments. However, our understanding of N2O reducers in aquatic systems is currently limited. This study investigated the relative abundance and diversity of nosZI- and nosZII-type N2O reducers in rivers and their impact on N2O emissions. Our findings revealed that stream sediments possess a high capacity for N2O reduction, surpassing N2O production under high N2O/NO3- ratio conditions. This study, along with others in freshwater systems, demonstrated that nosZI marginally dominates more often in rivers. While microbes containing either nosZI and nosZII were crucial in reducing N2O emissions, the net contribution of nosZII-containing microbes was more significant. This can be attributed to the nir gene co-occurring more frequently with the nosZI gene than with the nosZII gene. The diversity within each clade also played a role, with nosZII species being more likely to function as N2O sinks in streams with higher N2O concentrations. Overall, our findings provide a foundation for a better understanding of the biogeography of stream N2O reducers and their effects on N2O emissions.
Subject(s)
Bacteria , Nitrous Oxide , Rivers , Nitrous Oxide/metabolism , Rivers/microbiology , Rivers/chemistry , Bacteria/genetics , Bacteria/classification , Bacteria/metabolism , Geologic Sediments/microbiology , Oxidation-Reduction , Phylogeography , Phylogeny , MicrobiotaABSTRACT
There is growing evidence that the transformation products of emerging contaminants in foodstuffs may pose a health risk to humans. However, the exact identities, levels, and estimated dietary intake (EDI) of neonicotinoid transformation products in crops remain poorly understood. We established an extended suspect screening strategy to investigate neonicotinoid insecticides and their transformation products in retail cowpea from 11 cities in Hainan Province, China. Forty-nine transformation products were identified in retail cowpea, of which 22-36 were found in 98.6% of the samples. Notably, 31 new transformation products were derived from new processes or a combination of different transformation processes. The mean concentrations of neonicotinoids and nine of the transformation products (with authentic standards) were in the ranges of 0.0824-5.34 and 0.0636-1.50 ng/g, respectively. The cumulative EDIs of the quantified transformation products were lower than those of parent neonicotinoids with the exception of clothianidin desmethyl, which had a ratio of 1157%. However, the coexistence of the other 40 transformation products (without authentic standards) in cowpea suggested that the exposure risk from all of the transformation products might be higher. This study demonstrated that pesticide transformation products should be considered in food chain risk assessments and included in future regulatory management.
Subject(s)
Insecticides , Vigna , Humans , Neonicotinoids , Crops, Agricultural , China , Nitro CompoundsABSTRACT
Methane (CH4) is a potent greenhouse gas and its concentrations have tripled in the atmosphere since the industrial revolution. There is evidence that global warming has increased CH4 emissions from freshwater ecosystems1,2, providing positive feedback to the global climate. Yet for rivers and streams, the controls and the magnitude of CH4 emissions remain highly uncertain3,4. Here we report a spatially explicit global estimate of CH4 emissions from running waters, accounting for 27.9 (16.7-39.7) Tg CH4 per year and roughly equal in magnitude to those of other freshwater systems5,6. Riverine CH4 emissions are not strongly temperature dependent, with low average activation energy (EM = 0.14 eV) compared with that of lakes and wetlands (EM = 0.96 eV)1. By contrast, global patterns of emissions are characterized by large fluxes in high- and low-latitude settings as well as in human-dominated environments. These patterns are explained by edaphic and climate features that are linked to anoxia in and near fluvial habitats, including a high supply of organic matter and water saturation in hydrologically connected soils. Our results highlight the importance of land-water connections in regulating CH4 supply to running waters, which is vulnerable not only to direct human modifications but also to several climate change responses on land.
Subject(s)
Ecosystem , Methane , Rivers , Lakes/chemistry , Methane/analysis , Methane/metabolism , Rivers/chemistry , Wetlands , Global Warming/statistics & numerical data , Human ActivitiesABSTRACT
Constituents and functionality of urban inland waters are significantly perturbed by municipal sewage inputs and tailwater discharge from wastewater treatment plants. However, large knowledge gaps persist in understanding greenhouse gas dynamics in urban inland waters due to a lack of in situ measurements. Herein, via a 3-year field campaign (2018-2020), we report river and lake CO2 emission and related aquatic factors regulating the emission in the municipality of Beijing. Mean pCO2 (546 ± 481 µatm) in the two urban lakes was lower than global non-tropical freshwater lakes and CO2 flux in 47% of the lake observations was negative. Though average pCO2 in urban rivers (3124 ± 3846 µatm) was among the higher range of global rivers (1300-4300 µatm), average CO2 flux was much lower than the global river average (99.7 ± 147.5 versus 358.4 mmol m-2 d-1). The high pCO2 cannot release to the atmosphere due to the low gas exchange rate in urban rivers (average k600 of 1.3 ± 1.3 m d-1), resulting in low CO2 flux in urban rivers. Additionally, eutrophication promotes photosynthetic uptake and aquatic organic substrate production, leading to no clear relationships observed between pCO2 and phytoplankton photosynthesis or dissolved organic carbon. In consistence with the findings, CO2 emission accounted for only 32% of the total greenhouse gas (GHG) emission equivalence (CO2, CH4 and N2O) in Beijing waters, in contrast to a major role of anthropogenic CO2 to anthropogenic GHG in the atmosphere in terms of radiative forcing (66%). These results pointed to unique GHG emission profiles and the need for a special account of urban inland waters in terms of aquatic GHG emissions.
Subject(s)
Greenhouse Gases , Greenhouse Gases/analysis , Carbon Dioxide/analysis , Methane/analysis , Lakes , RiversABSTRACT
Heavy metals (HMs) pose ecological and resistome risks to aquatic systems. To efficiently develop targeted risk mitigation strategies, apportioning HM sources and assessing their source-oriented risks are essential. Although many studies have reported risk assessment and source apportionment of HMs, yet few have explored source-specific ecological and resistome risks associated with geochemical enrichment of HMs in aquatic environments. Therefore, this study proposes an integrated technological framework to characterize source-oriented ecological and resistome risks in the sediments of a plain river in China. Several geochemical tools quantitatively showed Cd and Hg had the highest pollution levels in the environment, with 19.7 and 7.5 times higher than their background values, respectively. Positive matrix factorization (PMF) and Unmix were comparatively used to apportion sources of HMs. Essentially, the two models were complementary and identified similar sources including industrial discharges, agricultural activities, atmospheric deposition and natural background, with contributions of 32.3-37.0%, 8.0-9.0%, 12.1-15.9% and 42.8-43.0%, respectively. To analyze source-specific ecological risks, the apportionment results were integratively incorporated into a modified ecological risk index. The results showed anthropogenic sources were the most significant contributors to the ecological risks. Particularly, industrial discharges majorly contributed high- (44%) and extremely high (52%) ecological risk for Cd, while agricultural activities posed a greater percentage of considerable-(36%) and high- (46%) ecological risk for Hg. Furthermore, the high-throughput sequencing metagenomic analysis identified abundant and diverse antibiotic resistance genes (ARGs), including some carbapenem-resistance genes and emerging genes such as mcr-type in the river sediments. Network and statistical analyses displayed significant correlations between ARGs and geochemical enrichment of HMs (ρ > 0.8; P-value <0.01), indicating their important impacts on resistome risks in the environment. This study provides useful insights into risk prevention and pollution control of HMs, and the framework can be made applicable to other rivers facing environmental challenges worldwide.
Subject(s)
Mercury , Metals, Heavy , Rivers/chemistry , Cadmium/analysis , Environmental Monitoring/methods , Metals, Heavy/analysis , Mercury/analysis , China , Risk Assessment , Anti-Bacterial Agents/analysis , Geologic Sediments/chemistryABSTRACT
Humic substances (HSs) play important roles in the transport and bioavailability of hydrophobic organic compounds (HOCs) in soils. The sorption of HOCs depends on the compositions and structures of HSs which may differ in different climatic zones, however, the sorption behavior of HOCs by HSs in soils from different climatic zones is poorly understood. In this study, different HS fractions (humic acids-HAs, fulvic acids-FAs and humin-HM) in soils from different climatic zones were extracted and used as sorbents for polycyclic aromatic hydrocarbons (PAHs). The results indicated that HSs (including HA, FA and HM fractions) from colder climatic zones contained more oxygen-containing functional groups and exhibited smaller molecular weight as well as higher aliphaticity and polarity than those from warmer climatic zones. The sorption affinity of HAs at the low given concentration (0.05 Sw) of naphthalene (Nap), phenanthrene (Phe), pyrene (Pyr) and benz(α)anthracene (BaA) from warmer climatic zones to colder ones increased from 26.3 to 43.9, from 36.7 to 114.0, from 125.8 to 388.8, and from 322.5 to 876.1, respectively, and the same trends were obtained for FAs and HM at the same PAH concentration. The results indicated that HSs from colder climatic zones showed higher sorption affinity than those from warmer climatic zones. Moreover, the weighted contributions of FAs, HAs and HM to the overall sorption from different climatic zones were 9.1-28.4%, 13.5-59.2% and 23.4-76.9%, respectively. This indicates FA fraction, a previously neglected component, is also an important contributor to binding PAHs in soils. This study suggests that the difference in sorption behaviors of HOCs to HSs among different climatic zones should be considered when predicting HOC fates and bioavailability in soils.
Subject(s)
Phenanthrenes , Polycyclic Aromatic Hydrocarbons , Soil Pollutants , Humic Substances/analysis , Soil/chemistry , Polycyclic Aromatic Hydrocarbons/analysis , Adsorption , Phenanthrenes/chemistry , Soil Pollutants/analysisABSTRACT
Erosion is the most widespread form of soil degradation and an important pathway of carbon transfer from land into aquatic systems, with significant impact on water quality and carbon cycle. However, it remains debatable whether erosion induces a carbon source or sink, and the fate of eroded soil carbon in aquatic systems remains poorly constrained. Here, we collect 41 representative soils from seven erosion-influenced basins and conduct microcosm simulation experiments to examine the fate of soil carbon under three different scenarios. We showed that soil carbon mineralization was generally promoted (by up to 10 times) in water under turbulence relative to in soils, but suppressed under static conditions upon entering into aquatic systems. Moreover, the enhancement of mineralization in turbulent systems is primarily related to soil aggregate content, while suppression in static systems positively relates to macromolecule abundance, indicating that soil geochemistry affects the magnitude of hydrodynamic effects on carbon mineralization. Random forest model further predicts that erosion may induce significant carbon sources in basins dominated by turbulent waters and aggregate-rich soils. Our findings demonstrate hydrodynamic and geochemical controls on soil carbon mineralization upon delivery into aquatic systems, which is a non-negligible part of the boundless carbon cycle and must be considered when making region-specific conservation strategies to reduce CO2 emissions from inland waters.
Subject(s)
Carbon , Soil , Soil/chemistry , Carbon/chemistry , Hydrodynamics , Carbon Cycle , Water QualityABSTRACT
Streams and rivers are important sources of nitrous oxide (N2 O), a powerful greenhouse gas. Estimating global riverine N2 O emissions is critical for the assessment of anthropogenic N2 O emission inventories. The indirect N2 O emission factor (EF5r ) model, one of the bottom-up approaches, adopts a fixed EF5r value to estimate riverine N2 O emissions based on IPCC methodology. However, the estimates have considerable uncertainty due to the large spatiotemporal variations in EF5r values. Factors regulating EF5r are poorly understood at the global scale. Here, we combine 4-year in situ observations across rivers of different land use types in China, with a global meta-analysis over six continents, to explore the spatiotemporal variations and controls on EF5r values. Our results show that the EF5r values in China and other regions with high N loads are lower than those for regions with lower N loads. Although the global mean EF5r value is comparable to the IPCC default value, the global EF5r values are highly skewed with large variations, indicating that adopting region-specific EF5r values rather than revising the fixed default value is more appropriate for the estimation of regional and global riverine N2 O emissions. The ratio of dissolved organic carbon to nitrate (DOC/NO3 - ) and NO3 - concentration are identified as the dominant predictors of region-specific EF5r values at both regional and global scales because stoichiometry and nutrients strictly regulate denitrification and N2 O production efficiency in rivers. A multiple linear regression model using DOC/NO3 - and NO3 - is proposed to predict region-specific EF5r values. The good fit of the model associated with easily obtained water quality variables allows its widespread application. This study fills a key knowledge gap in predicting region-specific EF5r values at the global scale and provides a pathway to estimate global riverine N2 O emissions more accurately based on IPCC methodology.
Subject(s)
Nitrates , Nitrous Oxide , Nitrous Oxide/analysis , Nitrates/analysis , Dissolved Organic Matter , Environmental Monitoring , RiversABSTRACT
SignificanceStream/river carbon dioxide (CO2) emission has significant spatial and seasonal variations critical for understanding its macroecosystem controls and plumbing of the terrestrial carbon budget. We relied on direct fluvial CO2 partial pressure measurements and seasonally varying gas transfer velocity and river network surface area estimates to resolve reach-level seasonal variations of the flux at the global scale. The percentage of terrestrial primary production (GPP) shunted into rivers that ultimately contributes to CO2 evasion increases with discharge across regions, due to a stronger response in fluvial CO2 evasion to discharge than GPP. This highlights the importance of hydrology, in particular water throughput, in terrestrial-fluvial carbon transfers and the need to account for this effect in plumbing the terrestrial carbon budget.
ABSTRACT
Streams and rivers emit substantial amounts of nitrous oxide (N2O) and are therefore an essential component of global nitrogen (N) cycle. Permafrost soils store a large reservoir of dormant N that, upon thawing, can enter fluvial networks and partly degrade to N2O, yet the role of waterborne release of N2O in permafrost regions is unclear. Here we report N2O concentrations and fluxes during different seasons between 2016 and 2018 in four watersheds on the East Qinghai-Tibet Plateau. Thawing permafrost soils are known to emit N2O at a high rate, but permafrost rivers draining the East Qinghai-Tibet Plateau behave as unexpectedly minor sources of atmospheric N2O. Such low N2O fluxes are associated with low riverine dissolved inorganic N (DIN) after terrestrial plant uptake, unfavorable conditions for N2O generation via denitrification, and low N2O yield due to a small ratio of nitrite reductase: nitrous oxide reductase in these rivers. We estimate fluvial N2O emissions of 0.432 - 0.463 Gg N2O-N yr-1 from permafrost landscapes on the entire Qinghai-Tibet Plateau, which is marginal (~0.15%) given their areal contribution to global streams and rivers (0.7%). However, we suggest that these permafrost-affected rivers can shift from minor sources to strong emitters in the warmer future, likely giving rise to the permafrost non-carbon feedback that intensifies warming.
ABSTRACT
Little is known about the exchange of gaseous nitrogen (N2) with the atmosphere from urban inland waters, which are characterized by low carbon-tonitrogen ratios and low nitrogen-tophosphorus ratios. Here, we studied diffusive nitrogen loss based on the measurement of dissolved N2 concentrations and related gene abundance of N2 production and fixation in rivers and lakes in the megacity of Beijing, China, between 2018 and 2020. The excess dissolved N2 (â³N2) ranged from -51.2 to 56.8 µmol L-1 (average - 0.03 ± 13.8 µmol L-1), and approximately 43% of the river samples and 72% of the lake samples being undersaturated with N2, suggesting that the lakes mainly acted as a role of N2 sink. The N2 removal fraction (â³N2/DIN, average 3.5 ± 4.3%) at the sites of rivers with positive â³N2 was lower than that in other rivers around the world. The average N2 flux (0.8 ± 23.9 mmol m-2 d-1) in the urban rivers was also lower than that in other rivers. The low carbon-tonitrogen ratios in Beijing inland waters are not beneficial for N2 production during denitrification, and low nitrogen-tophosphorus ratios potentially favor N2 fixation with a high abundance of the nitrogenase nifH gene in the sediment, resulting in low net N2 production. The traditional paradigm is that rivers constantly lose vast N to the atmosphere via denitrification and anammox, but this study indicates that urban inland rivers emit negligible N even under high nitrogen loading.
ABSTRACT
Inland waters are significant sources of nitrous oxide (N2O), a powerful greenhouse gas. However, considerable uncertainty exists in the estimates of N2O efflux from global inland waters due to a lack of direct measurements in urban inland waters, which are generally characterized by high carbon and nitrogen concentrations and low carbon-to-nitrogen ratios. Herein, we present direct measurements of N2O concentrations and fluxes in lakes and rivers of Beijing, China, during 2018-2020. N2O concentrations and fluxes in the waters of Beijing exceeded previous estimates of global rivers due to the high carbon and nutrient concentrations and high aquatic productivity. In contrast, the N2O emission factor (N2O-N/DIN, median 0.0005) was lower than global medians and the N2O yield (ΔN2O/(ΔN2O + ΔN2), average 1.6%) was higher than those typically observed in rivers and streams. The positive relationship between N2O emissions and denitrifying bacteria as well as the Michaelis-Menten relationship between N2O emissions and NO3--N concentrations suggested that bacteria control the net production of N2O in waters of Beijing with N saturation, leading to a low N2O emission factor. However, low carbon-to-nitrogen ratios are beneficial for N2O accumulation during denitrification, resulting in high N2O yields. This study demonstrates the significant N2O emissions and their distinctive patterns and controls in urban inland waters and suggests that N2O emission estimates based on nitrogen loads and simple emission factor values are not appropriate for urban inland water systems.
Subject(s)
Nitrous Oxide , Rivers , Beijing , China , Lakes , Nitrous Oxide/analysisABSTRACT
Carbon dioxide (CO2) evasion from inland waters is an important component of the global carbon cycle. However, it remains unknown how global change affects CO2 emissions over longer time scales. Here, we present seasonal and annual fluxes of CO2 emissions from streams, rivers, lakes, and reservoirs throughout China and quantify their changes over the past three decades. We found that the CO2 emissions declined from 138 ± 31 Tg C yr-1 in the 1980s to 98 ± 19 Tg C yr-1 in the 2010s. Our results suggest that this unexpected decrease was driven by a combination of environmental alterations, including massive conversion of free-flowing rivers to reservoirs and widespread implementation of reforestation programs. Meanwhile, we found increasing CO2 emissions from the Tibetan Plateau inland waters, likely attributable to increased terrestrial deliveries of organic carbon and expanded surface area due to climate change. We suggest that the CO2 emissions from Chinese inland waters have greatly offset the terrestrial carbon sink and are therefore a key component of China's carbon budget.
ABSTRACT
The evasions of methane (CH4) and carbon dioxide (CO2) from inland waters represent substantial fluxes of greenhouse gases into the atmosphere, offsetting a large part of the continental carbon sink. However, the CH4 and CO2 emissions from urban inland waters are less constrained. In particular, ebullitive CH4 emissions from these waters are poorly understood. Here, we measured the concentrations and fluxes of CH4 and CO2 in rivers and lakes in the megacity of Beijing, China, between 2018 and 2019. The CH4 concentration ranged from 0.08 to 70.2 µmol L-1 with an average of 2.5 ± 5.9 µmol L-1. The average CH4 ebullition was 11.3 ± 30.4 mmol m-2 d-1 and was approximately 6 times higher than the global average. The average total CH4 flux (14.2 ± 35.1 mmol m-2 d-1) was 3 times higher than the global average, with ebullition accounting for 80% of the flux. The high surface water CH4 concentrations and ebullitive fluxes were caused by high sediment organic carbon/dissolved organic carbon contents, high aquatic primary productivity and shallow water depths in the urban inland waters. The CH4 emissions accounted for 20% of CO2 emissions in terms of the carbon release and were 1.7 times higher in terms of CO2 equivalent emissions from Beijing inland waters. Furthermore, the CH4 ebullition and its contribution to the total carbon gas emissions increased exponentially with the water temperature, suggesting a positive feedback probably occurs between the greenhouse gas emissions from urban inland waters and climate warming. This study confirms the major role of CH4 ebullition from urban inland waters in the global carbon budget under the rapid progress of global urbanization.
Subject(s)
Greenhouse Gases , Beijing , Carbon Dioxide/analysis , China , Lakes , Methane/analysisABSTRACT
Groundwater discharge to river networks makes up a major source of riverine CO2 emission, available evidence however comes mainly from headwater streams which are directly connected to terrestrial ecosystems and spatially limited in terms of system size. Here relying on coupled water and CO2 mass balances, we quantified the groundwater-mediated CO2 input to the Yangtze River mainstem on an annual basis, where the mass balance of water provided physical constraints on CO2 exchange between the river and groundwater. A landscape topographic control of the groundwater-river interaction was proposed where mountain reaches preferentially receive water and CO2 discharge from the groundwater while plain alluvial reaches predominantly lose water to the aquifers. Groundwater CO2 inputs were however small in magnitude on all reaches (0.3-14% of the total CO2 emission and transport by the river) and unable to account for the discrepancy between surface evasion and internal metabolism in the river. Minor direct groundwater discharge to the reaches in comparison to smaller streams (negative to < 3.5% of the surface water flows) was concluded to be the main reason for low groundwater-sourced CO2 in the large river reaches.
ABSTRACT
Present-day estimations of global nitrogen loss (N-loss) are underestimated. Commonly, N-loss from rivers is thought to be caused by denitrification only in bed-sediments. However, coupled nitrification-denitrification occurring in overlying water with suspended sediments (SPS) where oxic and anoxic/low oxygen zones may coexist is ignored for N-loss in rivers. Here the Yellow and Yangtze Rivers were taken as examples to investigate the effect of SPS, which exists in many rivers of the world, on N loss through coupled nitrification-denitrification with nitrogen stable (15N) isotopic tracer simulation experiments and in-situ investigation. The results showed even when SPS was surrounded by oxic waters, there were redox conditions that transitioned from an oxic surface layer to anoxic layer near the particle center, enabling coupled nitrification-denitrification to occur around SPS. The production rate of 15N2 from 15NH4+-N (R15N2-production) increased with increasing SPS concentration ([SPS]) as a power function (R15N2-production=a·[SPS]b) for both the SPS-water and bed sediment-SPS-water systems. The power-functional increase of nitrifying and denitrifying bacteria population with [SPS] accounted for the enhanced coupled nitrification-denitrification rate in overlying water. SPS also accelerated denitrification in bed-sediment due to increased NO3- concentration caused by SPS-mediated nitrification. For these two rivers, 1gL-1 SPS will lead to N-loss enhancement by approximately 25-120%, and the enhancement increased with organic carbon content of SPS. Thus, we conclude that SPS in overlying water is a hot spot for nitrogen loss in river systems and current estimates of in-stream N-loss are underestimated without consideration of SPS; this may partially compensate for the current imbalance of global nitrogen inputs and sinks.
ABSTRACT
Many previous studies have used δ(15)N and δ(18)O of nitrate (δ(15)NNO3 and δ(18)ONO3) to determine the nitrate sources in rivers but were subject to substantial uncertainties and limitations, especially associated with evaluating the atmospheric contribution. The Δ(17)O of nitrate (Δ(17)ONO3) has been suggested as an unambiguous tracer of atmospheric NO3(-) and may serve as an additional nitrate source constraint. In the present study, triple nitrate isotopes (δ(15)NNO3, Δ(17)ONO3, and δ(18)ONO3) were used for the first time to assess the sources and sinks of nitrate in the Yellow River (YR) basin, which is the second longest river in China. Results showed that the Δ(17)ONO3 of the water from the YR ranged from 0 to 1.6 during two normal-water seasons. This suggested that unprocessed atmospheric nitrate accounted for 0-7% of the total nitrate in the YR. The corrected δ(15)NNO3 and δ(18)ONO3 values with atmospheric imprints being removed indicated that the main terrestrial sources of nitrate were sewage/manure effluents in the upstream of the YR and manure/sewage effluents and ammonium/urea-containing fertilizer in the middle and lower reaches which made comparable contributions to the nitrate. In addition, there was a significant positive relationship between δ(15)NNO3 and δ(18)ONO3 values of river water (p < 0.01) which may signal the presence of denitrification. This study indicates that the triple nitrate isotope method is useful for assessing the nitrate sources in rivers, especially for the measurements of atmospheric nitrate contribution.
Subject(s)
Nitrates/analysis , Nitrogen Isotopes/analysis , Oxygen Isotopes/analysis , Rivers/chemistry , Water Pollutants, Chemical/analysis , China , Denitrification , Environmental Monitoring/methods , Fertilizers , Manure , Models, Theoretical , SewageABSTRACT
High suspended sediment (SPS) concentration exists in many rivers of the world. In the present study, the effects of SPS concentration on denitrification were investigated in airtight chambers with sediment samples collected from the Yellow River which is the largest turbid river in the world. Results from the nitrogen stable ((15)N) isotopic tracer experiments showed that denitrification could occur on SPS in oxic waters and the denitrification rate increased with SPS concentration; this was probably caused by the presence of low-oxygen microsites in SPS. For the water systems with both bed-sediment and SPS, the denitrification kinetics fit well to Logistic model, and the denitrification rate constant increased linearly with SPS concentration (p < 0.01). The denitrification caused by the presence of SPS accounted for 22%, 38%, 53%, and 67% of the total denitrification in systems with 2.5, 8, 15, and 20 g L(-1) SPS, respectively. The activity of denitrifying bacteria in SPS was approximately twice that in bed-sediment, and the denitrifying bacteria population showed an increasing trend with SPS concentration in both SPS and bed-sediment, leading to the increase of denitrification rate with SPS concentration. Furthermore, the denitrification in bed-sediment was accelerated by increased diffusion of nitrate from overlying water to bed-sediment under agitation conditions, which accompanied with the presence of SPS. When with 8 g L(-1) SPS, approximately 66% of the increased denitrification compared to that without SPS was attributed to denitrification on SPS and 34% to agitation conditions. This is the first report of the occurrence of denitrification on SPS in oxic waters. The results suggest that SPS plays an important role in denitrification in turbid rivers; its effect on nitrogen cycle should be considered in future study.
Subject(s)
Denitrification , Geologic Sediments , Oxygen/chemistry , Rivers , Bacteria/genetics , Bacteria/metabolism , Base Sequence , DNA Primers , Polymerase Chain ReactionABSTRACT
The concentrations of black carbon (BC), total organic carbon (TOC) and polycyclic aromatic hydrocarbons (PAHs) have been determined in soils from urban and rural areas of Beijing. The rural area can be divided into plain and mountainous areas which are close to and relatively far from the urban area, respectively. Concentration of BC (5.83 ± 3.05 mg g⻹) and BC/TOC concentration ratio (0.37 ± 0.15) in Beijing's urban soil are high compared with that in world background soils and rural soils of Beijing, suggesting the urban environment to be an essential source and sink of BC. Concentration of BC in the urban area decreases from the inner city to exterior areas, which correlates with the urbanization history of Beijing and infers accumulation of BC in old urban soils. Black carbon in Beijing soils mainly comes from fossil fuel combustion, especially traffic emission. Median PAH concentration in the urban area (502 ng g⻹) is one order of magnitude higher than that in the rural plain (148 ng g⻹) and mountainous area (146 ng g⻹) where PAHs are supposed to mainly come from atmospheric deposition from the urban area. Concentrations of BC correlate significantly with those of PAHs (p < 0.01, except naphthalene) in the urban area and with those of heavier 4-, 5- and 6- ring PAHs (p < 0.01) in the adjacent rural plain area, while there is no significant correlation with any PAH in the farther rural mountainous area.