Eutrophication driven macrophyte-derived organic matter decomposition to methane emission relates to co-metabolism effect in freshwater sediments.

Lakes and wetlands play pivotal roles in global organic matter storage, receiving significant inputs of organic material. However, the co-metabolic processes governing the decomposition of these organic materials and their impact on greenhouse gas emissions remain inadequately understood. This study aims to assess the effects of mixed decomposition involving macrophytes and cyanobacteria on carbon emissions. A series of microcosms was established to investigate the decomposition of macrophyte residues and algae over a period of 216 days. A two-component kinetic model was utilized to estimate methane (CH4) production rates. Gas isotope technology was employed to discern the contributions of CH4 produced by macrophyte residues or algae. Quantitative PCR and analysis of 16S rRNA gene amplicons were employed to assess changes in functional genes and microbial communities. There were significant differences in the cumulative carbon release from the decomposition of different plant types due to the addition of carbon sources. After adding algae, the cumulative emission of CH4 increased significantly. The δ13C-CH4 partitioning indicated that CH4 originated exclusively from the fresh organic carbon of macrophyte residues, while it shifted to algae source after adding algae. The synergistic effect of the mixed decomposition on the CH4 emissions was greater than the sum of the individual decompositions. The microbial community richness was higher in the single plant residue treatment compared to the mixed treatment with algae addition, while microbial evenness in the sediment increased steadily in each treatment. Our findings emphasize the pronounced co-metabolic effect observed during the mixed decomposition of macrophytes and cyanobacteria.

Instability in a carbon pool driven by multiple dissolved organic matter sources in a eutrophic lake basin: Potential factors for increased greenhouse gas emissions.

Lakes serve as vital reservoirs of dissolved organic matter (DOM) and play pivotal roles in biogeochemical carbon cycles. However, the sources and compositions of DOM in freshwater lakes and their potential effects on lake sediment carbon pools remain unclear. In this study, seven inflowing rivers in the Lake Taihu basin were selected to explore the potential effects of multi-source DOM inputs on the stability of the lake sediment carbon pool. The results showed the high concentrations of dissolved organic carbon in the Lake Taihu basin, accompanied by a high complexity level. Lignins constituted the majority of DOM compounds, surpassing 40% of the total, while the organic carbon content was predominantly composed of humic acids (1.02-3.01 g kg-1). The high amounts of lignin oxidative cleavage led to CHO being the main molecular structure in the DOM of the seven rivers. The carbon constituents within the sediment carbon reservoir exhibited a positive correlation with dissolved CH4 and CO2, with a notable emphasis on humic acid and dissolved CH4 (R2 = 0.86). The elevated concentration of DOM, coupled with its intricate composition, contributed to the increases in dissolved greenhouse gases (GHGs). Experiments showed that the mixing of multi-source DOM can accelerate the organic carbon mineralization processes. The unit carbon emission efficiency was highest in the mixed group, reaching reached 160.9 µmol∙Cg-1, which also exhibited a significantly different carbon pool. The mixed decomposition of DOM from different sources influenced the roles of the lake carbon pool as source and sink, indicating that the multi-source DOM of this lake basin was a potential driving factor for increased carbon emissions. These findings have improved our understanding of the sources and compositions of DOM in lake basins and revealed their impacts on carbon emissions, thereby providing a theoretical basis for improving assessments of lake carbon emissions.

Space-for-time substitution leads to carbon emission overestimation in eutrophic lakes.

Lacustrine eutrophication is generally considered as an important contributor of carbon emissions to the atmosphere; however, there is still a huge challenge in accuracy estimating carbon emissions from lakes. To test the effect of widely used space-for-time substitution on lake carbon emissions, this study monitored different processes of carbon emissions, including the carbon production potential, dissolved carbon concentrations, and carbon release fluxes in eight lakes along the trophic gradients on a spatial scale and the typical eutrophic Lake Taihu for one year on a temporal scale. Eutrophication promoted carbon production potential, dissolved carbon concentrations, and carbon release fluxes, especially for CH4. Trophic lake index (TLI) showed positive correlations with the CH4 production potential, dissolved CH4 concentrations, and CH4 release fluxes, and also positive correlations with the CO2 production potential, dissolved CO2 concentrations, and CO2 release fluxes. The space-for-time substitution led to an overestimation for the influence of eutrophication on carbon emissions, especially the further intensification of lake eutrophication. On the spatial scale, the average CH4 production potential, dissolved CH4 concentrations and CH4 release fluxes in eutrophic lakes were 268.6, 0.96 µmol/L, and 587.6 µmol m-2·h-1, respectively, while they were 215.8, 0.79 µmol/L, and 548.6 µmol m-2·h-1 on the temporal scale. Obviously, CH4 and CO2 emissions on the spatial scale were significantly higher than those on the temporal scale in eutrophic lakes. The primary influencing factors were the seasonal changes in the physicochemical environments of lake water, including dissolved oxygen (DO) and temperature. The CH4 and CO2 release fluxes showed negative correlations with DO, while temperature displayed positive correlations, respectively. These results suggest that the effects of DO and temperature on lake carbon emissions should be considered, which may be ignored during the accurate assessment of lake carbon budget via space-for-time substitution in eutrophic lakes.

Dynamic sulfur-iron cycle promoted phosphorus mobilization in sediments driven by the algae decomposition.

Direct evidence of the algae bloom in eutrophic freshwater lakes on sulfur cycle and the subsequent iron oxide reduction and the iron oxides-bound phosphate (Fe-P) release in sediments is lacking. In this study, microcosms experiment was carried out to investigate the dynamic variations of S, Fe and P species in the water column and sediments as well as the sulfate reducing bacteria (SRB) abundance variation in the sediments during algae decomposition. The sulfate reduction was stimulated by the algae decomposition, which resulted in dramatic sulfate decline, sulfide increase and SRB growth. In addition, large amounts of acid volatile sulfide (AVS), pyrite sulfur (Pyrite-S) and elemental sulfur (S0) accumulated in the sediment. In particular, the contents of sedimentary Fe(II) and Pyrite-S in surface sediments continuously accumulated until the end of the experiment. Moreover, the terminal Fe-P content reduced by 35.4% compared with the initial concentration at high algae density group. These results suggested the irreversible reduction of iron oxides and revealed iron chemical reduction mediated by sulfide during algae decomposition. In addition, the connection of sulfur-iron cycle and the significant promotion of Fe-P mobilization in sediments was established, which should be paid more attention in the eutrophic freshwater ecosystems.

Unexpected increase of sulfate concentrations and potential impact on CH4 budgets in freshwater lakes.

The continuous increase in sulfate (SO42-) concentrations discharged by anthropogenic activities lacks insights into their dynamics and potential impact on CH4 budgets in freshwater lakes. Here we conducted a field investigation in the lakes along the highly developed Yangtze River basin, China, additionally, we analyzed long-term data (1950-2020) from Lake Taihu, a typical eutrophic lake worldwide. We observed a gradual increase in SO42- concentrations up to 100 mg/L, which showed a positive correlation with the trophic state of the lakes. The annual variations indicated that eutrophication intensified the fluctuation of SO42- concentrations. A random forest model was applied to assess the impact of SO42- concentrations on CH4 emissions, revealing a significant negative effect. Synchronously, a series of microcosms with added SO42- were established to simulate cyanobacteria decomposition processes and explore the coupling mechanism between sulfate reduction and CH4 production. The results showed a strong negative correlation between CH4 concentrations and initial SO42- levels (R2 = 0.83), indicating that higher initial SO42- concentrations led to lower final CH4 concentrations. This was attributed to the competition for cyanobacteria-supplied substrates between sulfate reduction bacteria (SRB) and methane production archaea (MPA). Our study highlights the importance of considering the unexpectedly increasing SO42- concentrations in eutrophic lakes when estimating global CH4 emission budgets.

Cyanobacteria decay alters CH4 and CO2 produced hotspots along vertical sediment profiles in eutrophic lakes.

Cyanobacteria-derived organic carbon has been reported to intensify greenhouse gas emissions from lacustrine sediments. However, the specific processes of CH4 and CO2 production and release from sediments into the atmosphere remain unclear, especially in eutrophic lakes. To investigate the influence of severe cyanobacteria accumulation on the production and migration of sedimentary CH4 and CO2, this study examined the different trophic level lakes along the middle and lower reaches of the Yangtze River. The results demonstrated that eutrophication amplified CH4 and CO2 emissions, notably in Lake Taihu, where fluxes peaked at 929.9 and 7222.5 µmol/m2·h, mirroring dissolved gas levels in overlying waters. Increased sedimentary organic carbon raised dissolved CH4 and CO2 concentrations in pore-water, with isotopic tracking showing cyanobacteria-derived carbon specifically elevated CH4 and CO2 in surface sediment pore-water more than in deeper layers. Cyanobacteria-derived carbon deposition on surface sediment boosted organic carbon and moisture levels, fostering an anaerobic microenvironment conducive to enhanced biogenic CH4 and CO2 production in surface sediments. In the microcosm systems with the most severe cyanobacteria accumulation, average CH4 and CO2 concentrations in surface sediments reached 6.9 and 2.3 mol/L, respectively, surpassing the 4.7 and 1.4 mol/L observed in bottom sediments, indicating upward migration of CH4 and CO2 hotspots from deeper to surface layers. These findings enhance our understanding of the mechanisms underlying lake sediment carbon emissions induced by eutrophication and provide a more accurate assessment of lake carbon emissions.

Response of sulfate concentration to eutrophication on spatio-temporal scale in freshwater lakes.

The dramatical increase of sulfur concentration in eutrophic lakes, especially sulfate (SO42-), has brought attention to the impact on the lake ecosystem; however, the mechanisms driving the intensification of eutrophication and the role of SO42- concentrations remain poorly understood. To assess the impact of eutrophication on SO42- dynamics in lakes, this study monitored SO42- concentrations in water and sediments across seven lakes with varying trophic statuses on a spatial scale, and in the eutrophic Lake Taihu over one year on a temporal scale, as well as a series of microcosms with different initial SO42- concentrations. Exogenous sulfur input is the primary driver of increased SO42- concentrations in lakes, the highest SO42- concentration in overlying water was 100 mg/L, as well as which reached 310.9 mg/L in sediment. The concurrent input of nutrients such as nitrogen and phosphorus exacerbated eutrophication, resulting in the destabilization of the sulfur cycle. Eutrophication promoted the SO42- concentration on the spatio-temporal scale, especially in sediment, and trophic lake index (TLI) showed a positive correlation with the SO42- in sediments (R2 = 0.99; 0.88). The SO42- concentration in water and TLI showed a nonlinear correlation on the temporal scale (R2 = 0.44), and showed a positive correlation on the spatial scale (R2 = 0.49). Microscopic experiments demonstrate that the anaerobic environment created by cyanobacteria decomposition induced sulfate reduction and significantly reduces SO42- concentrations. Concurrently, the anaerobic environment facilitates the coupling of iron reduction with sulfate reduction, leading to a substantial increase in Acid Volatile Sulfides (AVS) in the sediment. These findings reveal that eutrophication has a dual effect on the dynamic change of SO42- concentrations in overlying water, which is helpful to accurately evaluate and predict the change of SO42- concentrations in lakes.

Particulate organic carbon potentially increases methane emissions from oxic water of eutrophic lakes.

Lakes are hot spots for methane (CH4) emissions and particulate organic carbon (POC) production, which describes the methane paradox phenomenon. However, the current understanding of the source of POC and its effect on CH4 emissions during eutrophication remains unclear. In this study, 18 shallow lakes in different trophic states were selected to investigate the POC source and its contribution to CH4 production, particularly to reveal the underlying mechanisms of the methane paradox. The carbon isotopic analysis showed that the δ13Cpoc ranged from -30.28 ‰ to -21.14 ‰, indicating that cyanobacteria-derived carbon is an important source of POC. The overlying water was aerobic but contained high concentrations of dissolved CH4. Particularly, in hyper-eutrophic lakes, such as Lakes Taihu, Chaohu, and Dianshan, the dissolved CH4 concentrations were 2.11, 1.01, and 2.44 µmol/L, while the dissolved oxygen concentrations were 3.11, 2.92, and 3.17 mg/L, respectively. The intensified eutrophication increased the POC concentration, concomitantly promoting the dissolved CH4 concentration and the CH4 flux. These correlations revealed the role of POC in CH4 production and emission fluxes, particularly as a possible cause of the methane paradox, which is crucial for accurately evaluating the carbon budget and balance in shallow freshwater lakes.

Tidal variation and litter decomposition co-affect carbon emissions in estuarine wetlands.

Estuarine wetlands play important roles in the regional and global carbon cycle as well as greenhouse gas emissions; however, the driving factors and potential carbon emissions mechanisms are unclear. Here, the carbon emission fluxes were investigated in situ from different vegetated areas in the Chongming wetlands. The results showed that the highest methane (CH4) and carbon dioxide (CO2) emissions of 178.1 and 21,482.5 mg∙m-2∙min-1 were in Scirpus mariqueter and Phragmites australis dominated areas, respectively. A series of microcosms was strategically designed to simulate the influence of tidal variation on carbon emissions and the litter decomposition on daily- and monthly-timescales in estuarine wetlands. All added litter promoted CH4 and CO2 emissions from the wetland soils. The CH4 and CO2 emission fluxes of the S. mariqueter treatment were higher (367.7 vs. 108.4; 1607.9 vs. 1324.3 mg∙m-2∙min-1) than those of the P. australis treatment without tidal variation on a monthly timescale, due to the higher total organic carbon (TOC) content of S. mariqueter. The decomposition of litter also released a large amount of nutrients, which enhanced the abundance of methane-producing archaea (MPA) and methane-oxidizing bacteria (MOB). However, the tidal water level was negatively correlated with CH4 and CO2 emission fluxes. The CH4 and CO2 emission fluxes in the S. mariqueter treatment at the lowest tide were 556.02 and 604.99 mg∙m-2∙min-1, respectively. However, the CH4 and CO2 emission fluxes did not change significantly on the daily timescale in the S. mariqueter treatment without tidal variations. Therefore, the prolonged timescales revealed increases in litter decomposition but a decrease in the contribution of tidal variations to carbon emissions in estuarine wetlands. These findings provide a theoretical basis for evaluating the carbon cycle in estuarine wetlands.

Severe cyanobacteria accumulation potentially induces methylotrophic methane producing pathway in eutrophic lakes.

Although cyanobacteria blooms lead to an increase in methane (CH4) emissions in eutrophic lakes have been intensively studied, the methane production pathways and driving mechanisms of the associated CH4 emissions are still unclear. In this study, the hypereutrophic Lake Taihu, which has extreme cyanobacteria accumulation, was selected to test hypothesis of a potential methylotrophic CH4 production pathway. Field observation displayed that the CH4 emission flux from the area with cyanobacteria accumulation was 867.01 µg m-2·min-1, much higher than the flux of 3.44 µg m-2·min-1 in the non-cyanobacteria accumulation area. The corresponding abundance of methane-producing archaea (MPA) in the cyanobacteria-concentrated area was 77.33% higher than that in the non-concentrated area via RT-qPCR technologies. Synchronously, sediments from these areas were incubated in anaerobic bottles, and results exhibited the high CH4 emission potential of the cyanobacteria concentrated area versus the non-concentrated area (1199.26 vs. 205.76 µmol/L) and more active biological processes (CO2 emission, 2072.8 vs. -714.62 µmol/L). We also found evidence for the methylotrophic methane producing pathway, which contributed to the high CH4 emission flux from the cyanobacteria accumulation area. Firstly, cyanobacteria decomposition provided the prerequisite of abundant methyl thioether substances, including DMS, DMDS, and DMTS. Results showed that the content of methyl thioethers increased with the biomass of cyanobacteria, and the released DMS, DMDS, and DMTS was up to 96.35, 3.22 and 13.61 µg/L, respectively, in the highly concentrated 25000 g/cm3 cyanobacteria treatment. Then, cyanobacteria decomposition created anaerobic microenvironments (DO 0.06 mg/L and Eh -304.8Mv) for methylotrophic methane production. Lastly, the relative abundance of Methanosarcinales was increased from 7.67% at the initial stage to 36.02% at the final stage within a sediment treatment with 10 mmol/L N(CH3)3. Quantitatively, the proportion of the methylotrophic methane production pathway was as high as 32.58%. This finding is crucial for accurately evaluating the methane emission flux, and evaluating future management strategies of eutrophic lakes.

Increasing sulfate concentration and sedimentary decaying cyanobacteria co-affect organic carbon mineralization in eutrophic lake sediments.

Sulfate (SO42-) concentrations in eutrophic lakes are continuously increasing; however, the effect of increasing SO42- concentrations on organic carbon mineralization, especially the greenhouse gas emissions of sediments, remains unclear. Here, we constructed a series of microcosms with initial SO42- concentrations of 0, 30, 60, 90, 120, 150, and 180 mg/L to study the effects of increased SO42- concentrations, coupled with cyanobacterial blooms, on organic carbon mineralization in Lake Taihu. Cyanobacterial blooms promoted sulfate reduction and released a large amount of inorganic carbon. The SO42- concentrations in cyanobacteria treatments significantly decreased and eventually reached close to 0. As the initial SO42- concentration increased, the sulfate reduction rates significantly increased, with maximum values of 9.39, 9.44, 28.02, 30.89, 39.68, and 54.28 mg/L∙d for 30, 60, 90, 120, 150, and 180 mg/L SO42-, respectively. The total organic carbon content in sediments (51.16-52.70 g/kg) decreased with the initial SO42- concentration (R2 = 0.97), and the total inorganic carbon content in overlying water (159.97-182.73 mg/L) showed the opposite pattern (R2 = 0.91). The initial SO42- concentration was positively correlated with carbon dioxide (CO2) emissions (R2 = 0.68) and negatively correlated with methane (CH4) emissions (R2 = 0.96). The highest CO2 concentration and lowest CH4 concentration in the 180 mg/L SO42- treatment were 1688.78 and 1903 µmol/L, respectively. These biogeochemical processes were related to competition for organic carbon sources between sulfate reduction bacteria (SRB) and methane production archaea (MPA) in sediments. The abundance of SRB was positively correlated with the initial SO42- concentration and ranged from 6.65 × 107 to 2.98 × 108 copies/g; the abundance of MPA showed the opposite pattern and ranged from 1.99 × 108 to 3.35 × 108copies/g. These findings enhance our understanding of the effect of increasing SO42- concentrations on organic carbon mineralization and could enhance the accuracy of assessments of greenhouse gas emissions in eutrophic lakes.