A comprehensive conceptual framework for signaling in-lake CO2 through dissolved organic matter.

Organic carbon (C) and CO2 pools are closely interactive in aquatic environments. While there are strong indications linking freshwater CO2 to dissolved organic matter (DOM), the specific mechanisms underlying their common pathways remain unclear. Here, we present an extensive investigation from 20 subtropical lakes in China, establishing a comprehensive conceptual framework for identifying CO2 drivers and retrieving CO2 magnitude through co-trajectories of DOM evolution. Based on this framework, we show that lake CO2 during wet period is constrained by a combination of biogeochemical processes, while photo-mineralization of activated aromatic compounds fuels CO2 during dry period. We clearly determine that biological degradation of DOM governs temporal variations in CO2 rather than terrestrial C inputs within the subtropical lakes. Specifically, our results identify a shared route for the uptake of atmospheric polycyclic aromatic compounds and CO2 by lakes. Using machine learning, in-lake CO2 levels are well modelled through DOM signaling regardless of varying CO2 mechanisms. This study unravels the mechanistic underpinnings of causal links between lake CO2 and DOM, with important implications for understanding obscure aquatic CO2 drivers amidst the ongoing impacts of global climate change.

Air pollution control and carbon reduction policies: Assessing effectiveness in alleviating PM2.5-associated mortality in China.

To confront the challenges posed by air pollution and climate change, China has undertaken significant initiatives to develop strategies that address both issues concurrently. However, the health benefits of these initiatives have not been clearly articulated. In this study, the dynamic changes in health impacts under air pollution and carbon reduction actions in China are evaluated by employing the latest concentration-response models and projected PM2.5 concentrations under future scenarios. From 2020 to 2060, the enforcement of clean air and climate mitigation policies is expected to increase the percentage of the population living with PM2.5 concentrations meeting the 10 µg/m3 standard by 79 %. Without the implementation of relevant mitigation measures, PM2.5-associated deaths are projected to double due to an aging population. In comparison to the 2060 reference scenario, the joint implementation of clean air and carbon neutrality measures is expected to reduce nationwide PM2.5-associated mortality by 62 %, equivalent to 2.15 (95 % CI: 1.80-2.48) million deaths. Stringent pollution controls are crucial for reducing PM2.5-associated deaths before 2030, after which carbon neutrality actions become increasingly significant from 2030 to 2060. The challenges of mitigating future PM2.5-associated deaths vary greatly across regions, showing a critical response to pollution control and carbon reduction. The research proves the effectiveness of China's future air pollution control and carbon reduction policies in mitigating PM2.5-associated deaths.

Algae removal and algal organic matter chemistry modulated by KMnO4-PAC in simulated karst water.

In this study, we examined the modulation of algae removal and algal organic matter (AOM) chemistry by potassium permanganate and poly-aluminum chloride (KMnO4-PAC) in simulated karst water. Specifically, we verified the compositional changes of AOM sourcing from Chlorella sp. and Pseudanabaena sp. in response to the presence of divalent ions (Ca2+ and Mg2+). Aromatic protein and soluble microbial products were identified as the primary AOM components. Divalent ions accelerated dissolved organic carbon (DOC) and UV254 removal, particularly with Pseudanabaena sp. greater than Chlorella sp. (P < 0.05). Surface morphology analysis manifested that the removal of filamentous Pseudanabaena sp. was more feasible in comparison to globular Chlorella sp.. Our results highlight the significance of divalent ions in governing chemical behaviors and subsequent removal of both algae and AOM. This study upscales the understanding of the interactions among divalent ions, algae and AOM during preoxidation and coagulation process in algae-laden karst water.

Drivers of ozone-related premature mortality in China: Implications for historical and future scenarios.

Long-term exposure to ambient ozone (O3) poses a severe public health threat in China. However, the drivers of premature mortality caused by O3 pollution are still poorly constrained, despite being prerequisites for addressing the threat. Here, we demonstrate the contributions of historical and future changes in peak-season O3, population size, age structure, and baseline mortality to China's O3-related mortality using decomposition analysis. From 2013 to 2021, O3-related mortality decreased dramatically from 78.8 (40.8-124.6) to 68.7 (36.0-107.2) thousand, especially in densely populated areas with high pollution. Variations in peak-season O3, population size, age structure, and baseline mortality led to changes in O3-related mortality of +27.3 (14.8-41.3), +2.6 (1.4-4.1), +22.3 (11.5-35.2), and -40.3 (20.9-63.7) thousand, respectively. The influence of peak-season O3 on O3-related mortality shifted from positive during 2013-2019 (+8.4% per year) to negative during 2019-2021 (-8.8% per year), which highly regulated the interannual trend of mortality. From 2021 to 2035, O3-related mortality is expected to increase by 31% in the current context of peak-season O3 levels, primarily caused by increased aging. Even reducing peak-season O3 to the WHO interim target 1 (IT-1) would only reduce O3-related mortality by 3.9%, while a more rigorous standard (IT-2) would prevent 83.7% of mortality. These findings suggest that improving ambient O3 can lead to significant health benefits, but substantial mitigation strategies are merited given the future trend of population aging.

Land use and hydrological factors control concentrations and diffusive fluxes of riverine dissolved carbon dioxide and methane in low-order streams.

We analyzed the impacts of land use/land cover types on carbon dioxide (CO2) and methane (CH4) concentration and diffusion in 1st to 4th Strahler order tributaries of the Longchuan River to the upper Yangtze River in China by using headspace equilibration method and CO2SYS program. Field sampling and measurements were conducted during the dry and wet seasons from 2017 to 2019. The average of calculated CO2 partial pressure (pCO2, mean ± SD: 2389 ± 3220 µatm) by CO2SYS program was 1.9-fold higher than the value (mean ± SD: 1230 ± 1440 µatm) 10 years ago in the Longchuan River basin, where the urban land area increased by a factor of 7 times. Further analysis showed that corrected pCO2 by headspace method and dissolved CH4 (dCH4) decrease as the stream order and flow velocity increase. The pCO2 and dCH4 in the wet season was lower than that in the dry season. The explanatory ability of land use types on the variation of corrected pCO2 and dCH4 was stronger at the reach scale than at the riparian and catchment scales in two seasons. Urban land at reach scale further showed much higher explanation on corrected pCO2 and dCH4 than cropland, grassland and forest land in the wet season. The Longchuan River emits approximately 112.5 kt CO2-C and 1.0 kt CH4-C per year, being 1.7-fold of the total lateral export of dissolved inorganic and dissolved organic carbon (68.3 kt C y-1). The findings highlight the scale effects of land use on the observed seasonality in dissolved carbon gases in low-order streams.

Riverine nitrate source and transformation as affected by land use and land cover.

A mixed land use/land cover (LULC) catchment increases the complexity of sources and transformations of nitrate in rivers. Spatial paucity of sampling particularly low-resolution sampling in tributaries can result in a bias for identifying nitrate sources and transformations. In this study, high spatial resolution sampling campaigns covering mainstream and tributaries in combination with hydro-chemical parameters and dual isotopes of nitrate were performed to reveal spatio-temporal variations of nitrate sources and transformations in a river draining a mixed LULC catchment. This study suggested that point sources dominated the nitrate in the summer and winter, while non-point sources dominated the nitrate in the spring and autumn. A positive correlation was observed between proportions from sewage and land use index (LUI). However, negative correlations between soil nitrogen/nitrogen fertilizer and LUI were observed. With an increase of urban areas, the increased contribution from domestic sewage resulted in an increase of NO3- concentrations in rivers. Both urban and agricultural inputs should be considered in nitrate pollution management in a mixed LULC catchment. We concluded that the seasonal variations of nitrate sources were mainly affected by flow velocity conditions and agricultural activities, while spatial variations were mainly affected by LULC. In addition, we found a novel underestimation of dominated sources from Bayesian model because of mixing effect of isotope values from the tributaries to mainstream, however, high spatial resolution sampling can make up for this shortcoming. δ15N and δ18O values of nitrate indicated that nitrate originated from nitrification in soils. The nitrate concentrations and correlation between δ15N and 1/[NO3-] suggested little contribution of nitrate removal by denitrification. Thus, the nitrate reduction in the Yuehe River basin needs to be strengthened. The study provides new implications for estimation of nitrate sources and transformations and basis for nitrate reduction in the river with mixed LULC catchment.

Ultraviolet humic-like component contributes to riverine dissolved organic matter biodegradation.

Biological degradation of dissolved organic matter (DOM) regulates its structure and fate in river ecosystems. Previous views suggested that labile components were dominantly consumed by microbial metabolism. Here we provide new observations that a part of recalcitrant compounds largely contribute to riverine DOM biodegradation. The excitation-emission matrix fluorescent spectroscopy combined with peak picking and parallel factor analysis are used to explore component variability during DOM incubation. Humic-like and tryptophan-like DOM are the primary components of riverine DOM, with proportion contributions of 39%-82% and 16%-61% for % of the maximum fluorescence intensity, respectively. After 56 days of aerobic incubation in the dark, large amounts of tyrosine-like DOM generation are observed. Elevated temperature enhances the decomposition of ultraviolet humic-like substance and further stimulates labile DOM bio-mineralization into carbon dioxide. Meanwhile, averaged proportions of amino acid compositions (peak B and T) markedly increase (p < 0.05) as the humic-like compositions (peak A, M and C) decrease after DOM incubation, suggesting incomplete degradation of refractory DOM from high-molecular to low-molecular weight compounds. The findings support the new notion of the continuous DOM biodegradation in a mode as "steps by steps", contributing to a new understanding of carbon cycling for the UN Sustainable Development Goal.

Dynamics and internal links of dissolved carbon in a karst river system: Implications for composition, origin and fate.

Dissolved carbon (DC) deciphers biotic and abiotic processes in aquatic ecosystems, representing a critical component of global carbon cycling. However, underlying drivers of riverine DC dynamics and internal links have yet to be studied. Here, we investigated fluvial physicochemical characteristics, dissolved inorganic carbon (DIC) species, carbon dioxide (CO2) exchange, dissolved organic carbon (DOC) compositions and properties in a karst river system Qijiang, Southwest China. Carbonate dissolution combined with photosynthetic uptake could explain dynamics of DIC species. Carbon sequestration caused low-magnitude of partial pressure of aqueous CO2 (pCO2, 620.3 ± 1028.7 µatm) and water-air CO2 flux (F, 154.3 ± 772.6 mmol/m2/d), yielding an annual CO2 emission of 0.079 Tg CO2/y. Relatively high biological index (BIX, 0.77-0.96 on average) but low humification index (HIX, 0.67-0.78 on average) indicated notable autochthonous processes. Humic-like component was the predominant DOC, accounting for 39.0%-75.2% with a mean of 57.2% ± 6.17%. Meanwhile, tryptophan-like component (5.84% ± 2.31%) was also identified as collective DOC by parallel factor analysis (PARAFAC) across samples. Biological metabolism established internal linkages between DIC and DOC in the karst river system. Our findings highlighted biological process as a determinant for DC cycling in karst aquatic ecosystems.

Effect of dissolved organic matter and its fractions on disinfection by-products formation upon karst surface water.

In this study, disinfection by-products (DBP) formation from dissolved organic matter (DOM) and its fractions, including both hydrophilic and hydrophobic components, were investigated at a typical karst surface water. The subsequent DBP formation potential was evaluated by deducing chemical characteristics of DOM fractions and representative algal organic matter (Chlorella sp. AOM) under the influence of divalent ions (Ca2+ and Mg2+) via spectra analysis. Both terrigenous and autochthonous DOM performed as critical DBP precursors, and DBP formation patterns were tightly correlated to organic matter chemical variations. DBP formation was significantly higher in drought period compared to that in wet period (P < 0.05). Particularly, trichloromethane (TCM) and dichloroacetonitrile (DCAN) showed distinct formation patterns compared to the scenarios in non-karst water. For DOM fractions, hydrophobic components showed higher DBP formation compared to hydrophilic counterparts, hydrophilic neutral enriched more reactive organic nitrogen for N-DBPs production. It was preferable to enrich humic-like substances after Ca2+ and Mg2+complexation in Chlorella sp. AOM, TCM formation increased whereas DCAN production remained unchanged in the presence of divalent ions. This study innovatively provided a linkage between chemical characteristics of DOM and understanding of DBP formation in karst surface water.

[Dissolved Organic Matter Component and Source Characteristics of the Metropolitan Lakes and Reservoirs in a Typical Karst Region].

In order to explore dissolved organic matter (DOM) components and their origins in metropolitan lakes and reservoirs in the karst region, the typical Hongfeng Lake, Baihua Lake, Songbaishan Reservoir, and Aha Reservoir were investigated in Guiyang City. Surface water parameters, including dissolved organic carbon (DOC), chlorophyll a (Chla), and optical parameters (a254, a280, a350, E2:E3, S275-295, FI, ß:α, BIX, and HIX) were analyzed. Fluorescence peaks (B, T, A, M, C, D, and N) and three-dimensional matrix fluorescence with parallel factor analysis (EEM-PARAFAC) were employed to explain distinct DOM abundances and proportions. Meanwhile, Spearman's correlation coefficients and principal component analysis (PCA) were used to decipher parameter types and primary environmental processes. The results showed that aquatic ρ(DOC) and ρ(Chla) ranged between 4.24-11.9 mg·L-1 and 0.32-19.7 µg·L-1, respectively. High humic-like (a254) and protein DOM (a280) were observed in the Songbaishan Reservoir, resulting in higher DOM molecular weight when compared to that in other lakes and reservoirs. Surface water DOM mainly contained visible-light humic-like (23.8%-46.9%) and terrestrial fulvic-like components (17.6%-28.4%). High FI, ß:α, and BIX but low HIX values in this study suggested that endogenous inputs largely contributed to aquatic DOM. Aquatic DOM component and source characteristics were significantly correlated with each other. Furthermore, inputs of humic-like DOM and microbial metabolism, as well as coupled carbonate dissolution and photosynthesis, drove dynamic DOM behaviors in the karst lakes and reservoirs.

[Water-air Carbon Dioxide Exchange and Nutritional Controls in a Typical Karst River].

To explore water-air carbon dioxide (CO2) exchange and its nutritional controls in karst rivers, water sampling and analyses were conducted in the Furong River as a representative karst river system. Regional hydrometeorological characteristics, carbonate system parameters, total organic carbon (TOC), nutrients and their stoichiometric ratios, and the riverine pressure of aqueous CO2 (pCO2) and its couplings to trophic status were analyzed. The results showed that gas transfer velocity of CO2 (k) varied between 2.71 and 13.0 m·d-1. Riverine pCO2 varied from 78.5 Pa to 21491.2 Pa and was significantly higher in the tributaries than the main stem. Riverine TOC, total nitrogen (TN), and total phosphorus (TP) concentrations were (302.8±50.1), (128.9±67.9), and (0.65±0.98) µmol·L-1, respectively, demonstrating the trophic status of P-limitation. Riverine pCO2 was tightly linked to P-related parameters, suggesting that in-situ metabolism triggered aquatic CO2 supersaturation. Water-air CO2 flux (F) averaged (534.5±801.4) mmol·(m2·d)-1 in the Furong River, which is higher than most of the world's rivers, and thus indicates high potential CO2 emissions.

Seasonal variations of water quality response to land use metrics at multi-spatial scales in the Yangtze River basin.

Land use pattern is increasingly regarded as an important determinant of environmental quality and regional ecosystems. Understanding the correlation between land use metrics and water quality is essential to improve water pollution prediction and provide guidance for land use planning. Here, we examined the land use metrics and water quality parameters (i.e., dissolved oxygen, DO; pH; ammonia nitrogen NH4+-N; permanganate index, CODMn), as well as their relationships in the Yangtze River basin. The DO and pH exhibited the notable spatio-temporal variability, suggesting that anthropogenic land uses (farmland and urban land) greatly impacted riverine water quality. The catchment and riparian scales respectively showed a high potential in explaining water quality in the dry and wet seasons. The land use metrics were tightly linked to water quality in the dry season, indicating that intensive farming activities led to high loadings of agriculture-related chemicals and thus water quality deterioration. Our results provided useful information regarding riverine water quality response to land use metrics at multi-spatial scales.

Linking riverine partial pressure of carbon dioxide to dissolved organic matter optical properties in a Dry-hot Valley Region.

The mineralization of dissolved organic matter (DOM) can partially explain riverine carbon dioxide (CO2) emissions to the atmosphere. However, little is known about how the DOM origin and composition drive CO2 partial pressures (pCO2). Here, we reveal links between aquatic pCO2, DOM optical parameters (a254, a350 and S275-295 and S350-400) and nutrients in a subtropical river in China's Dry-hot Valley Region. Biodegradation preferentially decomposed low molecular weight (LMW) DOMs, increasing high molecular weight (HMW) DOMs along the main stem. pCO2 was positively correlated with aromatic and lignin compounds, but negatively correlated with DOM molecular weight. Aquatic respiration of DOMs largely explained the pCO2 levels in the drought period, while terrestrial inputs were a pCO2 source in the initial-wet period. Our results illustrate how both DOM concentrations and speciation can explain pCO2 distribution and sources in rivers.

[Water-Air Interface CO2 Exchange Flux of Typical Lakes in a Mountainous Area of the Western Chongqing and Their Influencing Factors].

To examine the mountainous lake CO2 evasion in Southwest China, partial pressures of carbon dioxide[p(CO2)] and the CO2 exchange flux[F(CO2)] via the water-air interface of nine mountainous lakes in Chongqing, China, have been studied in summer using the thin boundary layer model (TBL) and floating chambers. Key water quality parameters were concomitantly measured. The results indicate that the pCO2 in the mountainous lakes in western Chongqing ranges from 2.1 to 45.0 Pa, with a mean value of (18.1±12.1) Pa. The mean CO2 fluxes calculated by the TBL model and chamber method are (-8.0±2.9), (-3.4±3.6), and (-7.1±22.3) mmol·(m2·d)-1, respectively. The p(CO2) and F(CO2) have positive correlations with the wind speed and ORP but negative correlations with the pH. Our study indicates that mountainous lakes are atmospheric sinks of CO2 and the TBL model should be cautiously adopted.

Optimization of Malachite Green Removal from Water by TiO2 Nanoparticles under UV Irradiation.

TiO2 nanoparticles with surface porosity were prepared by a simple and efficient method and presented for the removal of malachite green (MG), a representative organic pollutant, from aqueous solution. Photocatalytic degradation experiments were systematically conducted to investigate the influence of TiO2 dosage, pH value, and initial concentrations of MG. The kinetics of the reaction were monitored via UV spectroscopy and the kinetic process can be well predicted by the pseudo first-order model. The rate constants of the reaction kinetics were found to decrease as the initial MG concentration increased; increased via elevated pH value at a certain amount of TiO2 dosage. The maximum efficiency of photocatalytic degradation was obtained when the TiO2 dosage, pH value and initial concentrations of MG were 0.6 g/L, 8 and 10−5 mol/L (M), respectively. Results from this study provide a novel optimization and an efficient strategy for water pollutant treatment.

Electrokinetic-Fenton remediation of organochlorine pesticides from historically polluted soil.

Soil contamination by persistent organic pollutants (POPs) poses a great threat to historically polluted soil worldwide. In this study, soils were characterized, and organochlorine pesticides contained in the soils were identified and quantified. Individual electrokinetic (IE), EK-Fenton-coupled technologies (EF), and enhanced EK-Fenton treatment (E-1, E-2, and E-3) were applied to remediate soils contaminated with hexachloro-cyclohexane soprocide (HCH) and dichloro-diphenyl-trichloroethane (DDT). Variation of pH, electrical conductivity, and electroosmotic flow was evaluated during the EK-Fenton process. The IE treatment showed low removal efficiency for HCHs (30.5%) and DDTs (25.9%). In the EF treatment, the highest removal level (60.9%) was obtained for α-HCH, whereas P,P-DDT was the lowest (40.0%). Low solubility of pollutants impeded the HCH and DDT removal. After enhanced EK-Fenton treatment, final removal of pollutants decreased as follows: ß-HCH (82.6%) > γ-HCH (81.6%) > α-HCH (81.2%) > δ-HCH (80.0%) > P,P-DDD (73.8%) > P,P-DDE (73.1%) > P,P-DDT (72.6%) > O,P-DDT (71.5%). The results demonstrate that EK-Fenton is a promising technology for POP removal in historically polluted soil.

Heavy metals in soils of Hechuan County in the upper Yangtze (SW China): Comparative pollution assessment using multiple indices with high-spatial-resolution sampling.

In order to assess heavy metals (HMs) in soils of the upper Yangtze Basin, a very high-spatial-resolution sampling (582 soil samples) was conducted from Hechuan County, an important agricultural practice area in the Southwest China. Multiple indices including geoaccumulation index (Igeo), enrichment factor (EF), sediment pollution index (SPI) and risk index (RI), as well as multivariate statistics were employed for pollution assessment and source identification of HMs in soils. Our results demonstrated that the averages of eight HMs decreased in the following order: Zn (82.8 ± 15.9) > Cr (71.6 ± 12.2) > Ni (32.1 ± 9.89) > Pb (27.6 ± 13.8) > Cu (25.9 ± 11.8) > As (5.48 ± 3.42) > Cd (0.30 ± 0.077) > Hg (0.082 ± 0.092). Averages of HMs except Cd were lower than threshold value of Environmental Quality Standard for Soils, while 43% of total samples had Cd concentration exceeding the national standard, 1% of samples for Hg and 5% samples for Ni, moreover, Cd and Hg averages were much higher than their background levels. Igeo and EF indicated that their levels decreased as follows: Cd > Hg > Zn > Pb > Ni > Cu > Cr > As, with moderate enrichments of Cd and Hg. RI indicated that 61.7% of all samples showed moderate risk, while 6.5% of samples with greater than considerable risk due to human activities should be paid more attention. Multivariate analysis showed lithogenic source of Cu, Cr, Ni and Zn, while Cd and Hg were largely contributed by anthropogenic activities such as agricultural practices. Our study would be helpful for improving soil environmental quality in SW, China, as well as supplying modern approaches for other areas with soil HM pollution.