Pub Date : 2024-10-16DOI: 10.1016/j.watres.2024.122644
Jinyue Jiang, Lin Du, Buchun Si, Harshal D. Kawale, Zixin Wang, Sabrina Summers, Juan A. Lopez-Ruiz, Shuyun Li, Yuanhui Zhang, Zhiyong Jason Ren
The global shift toward net-zero emissions necessitates resource recovery from wet waste. In this study, we demonstrate the first feasibility of combining pilot-scale microbial electrolytic cells (MECs) with hydrothermal liquefaction (HTL) for simultaneous post-hydrothermal liquefaction wastewater (PHW) treatment and efficient hydrogen (H₂) production to meet biocrude upgrading requirements. Long-term single reactor operation revealed that fixed anode potential enabled rapid startup, and low catholyte pH and high salinity were effective in suppression of cathodic methanogenesis and acetogenesis – resulting in high current density of 16.6 A m−2 and 9.3 A m−2 when feeding synthetic wastewater and PHW respectively. Additionally, the anode biofilm exhibited spatial variations in response to local environmental conditions. Onsite parallel or serial operations of multiple MECs showed good performance using actual PHW with a record-high H2 production rate of 0.5 L LR day−1 for MEC over 10 liters scale, and the optimal chemical oxygen demand (COD)-to-H2 yield reached 0.127 kg-H2 per kg-COD, supporting a self-sufficient, closed-loop upgrade to jet fuel.
{"title":"Pilot Microbial Electrolysis Cell Closes the Hydrogen Loop for Hydrothermal Wet Waste Conversion to Jet Fuel","authors":"Jinyue Jiang, Lin Du, Buchun Si, Harshal D. Kawale, Zixin Wang, Sabrina Summers, Juan A. Lopez-Ruiz, Shuyun Li, Yuanhui Zhang, Zhiyong Jason Ren","doi":"10.1016/j.watres.2024.122644","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122644","url":null,"abstract":"The global shift toward net-zero emissions necessitates resource recovery from wet waste. In this study, we demonstrate the first feasibility of combining pilot-scale microbial electrolytic cells (MECs) with hydrothermal liquefaction (HTL) for simultaneous post-hydrothermal liquefaction wastewater (PHW) treatment and efficient hydrogen (H₂) production to meet biocrude upgrading requirements. Long-term single reactor operation revealed that fixed anode potential enabled rapid startup, and low catholyte pH and high salinity were effective in suppression of cathodic methanogenesis and acetogenesis – resulting in high current density of 16.6 A m<sup>−2</sup> and 9.3 A m<sup>−2</sup> when feeding synthetic wastewater and PHW respectively. Additionally, the anode biofilm exhibited spatial variations in response to local environmental conditions. Onsite parallel or serial operations of multiple MECs showed good performance using actual PHW with a record-high H<sub>2</sub> production rate of 0.5 L L<sub>R</sub> day<sup>−1</sup> for MEC over 10 liters scale, and the optimal chemical oxygen demand (COD)-to-H<sub>2</sub> yield reached 0.127 kg-H<sub>2</sub> per kg-COD, supporting a self-sufficient, closed-loop upgrade to jet fuel.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444305","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-16DOI: 10.1016/j.watres.2024.122645
Tianhong Tu, Le Li, Wenkai Li, Shan Zhang, Hui Zhong, Gang Ge, Lan Wu, Yantian Ma
Phosphorus (P) is a limiting factor in fresh waters and is also the main cause of water eutrophication and deterioration, However, the practical effect of elevated P level on bacterioplankton is less evaluated. In this study, we investigated the bacterioplankton in a 96 hours microcosm experiment with P additions in two forms (organic/inorganic P, OP/IP) and three levels (final conc., 0.040, 0.065 and 0.125 g/L), aiming to find out the response pattern of bacterioplankton in coping with the increasing P levels. Results showed a more dramatic change of water properties and bacterioplankton between P forms (OP and IP) than among the addition levels, and a more remarkable effect of OP addition than the IP. Both OP and IP treatments significantly decreased the water pH, dissolved oxygen (DO), Electrical Conductivity (EC), Nitrate Nitrogen (NO3--N) and Total Organic Carbon (TOC), and reduced the α-diversity of bacterioplankton and relative abundance of Cyanobacteria, but increased the abundance of Proteobacteria. The IP addition decreased Actinobacteria abundance (especially for HgcI) and showed higher denitrification potentials, while the OP addition depressed the Bateroidota and exhibited lowed methylotrophic functions, but such trends decreased with increasing addition concentrations. The network analysis showed that both IP and OP additions increased the proportion of positively correlated edges and reduced the network complexity and stability, but the OP network was more stable than the IP network. The study clarifies the response pattern of bacterioplankton to the P input with different forms and levels, and deepens our understanding of the eutrophication process, which provides a scientific basis for the management and control of freshwater lakes facing eutrophication.
磷(P)是淡水中的限制因子,也是水体富营养化和恶化的主要原因。在本研究中,我们在一个 96 小时的微观世界实验中,以两种形式(有机/无机磷,OP/IP)和三种水平(最终浓度,0.040、0.065 和 0.125 克/升)添加磷,对浮游细菌进行了调查,旨在找出浮游细菌在应对磷含量增加时的反应模式。结果表明,不同磷形式(OP 和 IP)之间水质和浮游细菌的变化比不同添加水平之间的变化更剧烈,OP 的添加效果比 IP 更显著。OP 和 IP 处理都明显降低了水的 pH 值、溶解氧(DO)、电导率(EC)、硝酸盐氮(NO3--N)和总有机碳(TOC),减少了浮游细菌的α-多样性和蓝藻的相对丰度,但增加了变形菌的丰度。添加 IP 会降低放线菌的丰度(尤其是 HgcI),并显示出较高的反硝化潜力,而添加 OP 则会抑制类蝠鲼的生长,并显示出较低的养甲功能,但这种趋势会随着添加浓度的增加而减弱。网络分析显示,添加 IP 和 OP 都增加了正相关边的比例,降低了网络的复杂性和稳定性,但 OP 网络比 IP 网络更稳定。该研究阐明了不同形式和水平的浮游细菌对P输入的响应模式,加深了对富营养化过程的认识,为面临富营养化的淡水湖泊的管理和控制提供了科学依据。
{"title":"Different patterns of bacterioplankton in response to inorganic and organic phosphorus inputs in freshwater lakes - a microcosmic study","authors":"Tianhong Tu, Le Li, Wenkai Li, Shan Zhang, Hui Zhong, Gang Ge, Lan Wu, Yantian Ma","doi":"10.1016/j.watres.2024.122645","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122645","url":null,"abstract":"Phosphorus (P) is a limiting factor in fresh waters and is also the main cause of water eutrophication and deterioration, However, the practical effect of elevated P level on bacterioplankton is less evaluated. In this study, we investigated the bacterioplankton in a 96 hours microcosm experiment with P additions in two forms (organic/inorganic P, OP/IP) and three levels (final conc., 0.040, 0.065 and 0.125 g/L), aiming to find out the response pattern of bacterioplankton in coping with the increasing P levels. Results showed a more dramatic change of water properties and bacterioplankton between P forms (OP and IP) than among the addition levels, and a more remarkable effect of OP addition than the IP. Both OP and IP treatments significantly decreased the water pH, dissolved oxygen (DO), Electrical Conductivity (EC), Nitrate Nitrogen (NO<sub>3</sub><sup>-</sup>-N) and Total Organic Carbon (TOC), and reduced the α-diversity of bacterioplankton and relative abundance of Cyanobacteria, but increased the abundance of Proteobacteria. The IP addition decreased Actinobacteria abundance (especially for HgcI) and showed higher denitrification potentials, while the OP addition depressed the Bateroidota and exhibited lowed methylotrophic functions, but such trends decreased with increasing addition concentrations. The network analysis showed that both IP and OP additions increased the proportion of positively correlated edges and reduced the network complexity and stability, but the OP network was more stable than the IP network. The study clarifies the response pattern of bacterioplankton to the P input with different forms and levels, and deepens our understanding of the eutrophication process, which provides a scientific basis for the management and control of freshwater lakes facing eutrophication.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439919","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Construction of cascade reservoirs has altered nutrient dynamics and biogeochemical cycles, thereby influencing the composition and productivity of river ecosystems. The Lancang River (LCR), characterized by its cascade reservoir system, presents uncertainties in nitrogen transport and nitrate transformation mechanisms. Herein, we conducted monthly monitoring of hydrochemistry and multiple stable isotopes (δ15N-NO3-, δ18O-NO3-, δ18O-H2O, δD-H2O) throughout 2019 in both the natural river reach (NRR) and cascade reservoirs reach (CRR) of the LCR. Through the monthly detection of nitrogen forms and runoff in the import (M2) and export (M9) section, the average annual retention ratios for Total nitrogen (TN), Nitrate nitrogen (NO3--N), Particulate Nitrogen (PN) and Ammonium Nitrogen (NH4+-N) were about -35%, -53%, 48% and -65%, respectively. The retention rates were positively correlated with hydraulic retention time and negatively correlated with reservoir age, especially in the flood season. Compared to the NRR, the reservoir had significantly affected the nitrogen transport characteristics, especially for the large reservoirs (like Xiaowan and Nuozhadu), which enhanced phytoplankton uptake of NO3--N to form PN capabilities in the lentic environment and subsequently to precipitate or intercept it at the reservoir. This led to the overall decreasing trend of TN and PN concentrations along the CRR. The Bayesian stable isotope model quantified NO3--N sources from the NRR to the CRR. During this transition, soil nitrogen (SN) ratios decreased from 69.3% to 61.8%, while Manure & sewage (M&S) increased from 24.0% to 31.3%. Anthropogenic and natural factors, including urban sewage discharge, population density, and precipitation, were selected as key predictor variables. The eXtreme Gradient Boosting (XGBoost) model exhibited superior predictive performance for NO3--N concentrations, achieving an R2 of 0.70. These findings deepen our understanding of the impact of reservoirs on river ecology.
{"title":"Deciphering the impact of cascade reservoirs on nitrogen transport and nitrate transformation: Insights from multiple isotope analysis and machine learning","authors":"Yufei Bao, Yuchun Wang, Mingming Hu, Peng Hu, Nanping Wu, Xiaodong Qu, Xiaobo Liu, Wei Huang, Jie Wen, Shanze Li, Meng Sun, Qian Zhang","doi":"10.1016/j.watres.2024.122638","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122638","url":null,"abstract":"Construction of cascade reservoirs has altered nutrient dynamics and biogeochemical cycles, thereby influencing the composition and productivity of river ecosystems. The Lancang River (LCR), characterized by its cascade reservoir system, presents uncertainties in nitrogen transport and nitrate transformation mechanisms. Herein, we conducted monthly monitoring of hydrochemistry and multiple stable isotopes (δ<sup>15</sup>N-NO<sub>3</sub><sup>-</sup>, δ<sup>18</sup>O-NO<sub>3</sub><sup>-</sup>, δ<sup>18</sup>O-H<sub>2</sub>O, δD-H<sub>2</sub>O) throughout 2019 in both the natural river reach (NRR) and cascade reservoirs reach (CRR) of the LCR. Through the monthly detection of nitrogen forms and runoff in the import (M2) and export (M9) section, the average annual retention ratios for Total nitrogen (TN), Nitrate nitrogen (NO<sub>3</sub><sup>-</sup>-N), Particulate Nitrogen (PN) and Ammonium Nitrogen (NH<sub>4</sub><sup>+</sup>-N) were about -35%, -53%, 48% and -65%, respectively. The retention rates were positively correlated with hydraulic retention time and negatively correlated with reservoir age, especially in the flood season. Compared to the NRR, the reservoir had significantly affected the nitrogen transport characteristics, especially for the large reservoirs (like Xiaowan and Nuozhadu), which enhanced phytoplankton uptake of NO<sub>3</sub><sup>-</sup>-N to form PN capabilities in the lentic environment and subsequently to precipitate or intercept it at the reservoir. This led to the overall decreasing trend of TN and PN concentrations along the CRR. The Bayesian stable isotope model quantified NO<sub>3</sub><sup>-</sup>-N sources from the NRR to the CRR. During this transition, soil nitrogen (SN) ratios decreased from 69.3% to 61.8%, while Manure & sewage (M&S) increased from 24.0% to 31.3%. Anthropogenic and natural factors, including urban sewage discharge, population density, and precipitation, were selected as key predictor variables. The eXtreme Gradient Boosting (XGBoost) model exhibited superior predictive performance for NO<sub>3</sub><sup>-</sup>-N concentrations, achieving an R<sup>2</sup> of 0.70. These findings deepen our understanding of the impact of reservoirs on river ecology.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439698","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-15DOI: 10.1016/j.watres.2024.122630
Xuecong Qian, Shilong Wang, Haijun Cheng, Luwei Li, Yun Liu, Jinhao Duan, Da Wang, Jun Ma
Fe(II) and Mn(II) are abundant in groundwater and require operationally simple and efficient method to remove in drinking water treatment. The rapid oxidation of Mn(II) is essential in water treatment. This study investigates the efficiency of Mn(II) oxidation by free chlorine in the presence of Fe(II). The results demonstrate that the presence of Fe(II) significantly accelerates the oxidation rate of Mn(II) by free chlorine under neutral and alkaline conditions. The rapid oxidation of Fe(II) by free chlorine and the presence of Mn(II) promote the formation of in situ Mn(II)-doped ferrihydrite. Kinetic modeling and characterization of Fe(III) oxides confirm that the heterogeneous catalytic effect of the Mn(II)-doped ferrihydrite, rather than manganese oxides or their coupled catalytic effect, is responsible for the enhanced oxidation rates. The doped Mn(II) substitutes the tetrahedral Fe(III) ions in the ferrihydrite, introducing additional negative charges at the doped sites. The increased charge enhances Mn(II) adsorption and lowers its redox potential, thereby accelerating Mn(II) oxidation rate through direct electron transfer with adjacent free chlorine. Additionally, the lepidocrocite formed by the reaction between Fe(II) and dissolved oxygen significantly impedes the catalytic performance. These findings provide new insights into the catalytic co-oxidation mechanism of Fe(II) and Mn(II), and help the optimization of water treatment engineering practices.
{"title":"Catalytic Oxidation of Mn(II) in the Co-presence of Fe(II) by Free Chlorine: Significance of In Situ Formed Mn(II)-Doped Fe(III) Oxides","authors":"Xuecong Qian, Shilong Wang, Haijun Cheng, Luwei Li, Yun Liu, Jinhao Duan, Da Wang, Jun Ma","doi":"10.1016/j.watres.2024.122630","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122630","url":null,"abstract":"Fe(II) and Mn(II) are abundant in groundwater and require operationally simple and efficient method to remove in drinking water treatment. The rapid oxidation of Mn(II) is essential in water treatment. This study investigates the efficiency of Mn(II) oxidation by free chlorine in the presence of Fe(II). The results demonstrate that the presence of Fe(II) significantly accelerates the oxidation rate of Mn(II) by free chlorine under neutral and alkaline conditions. The rapid oxidation of Fe(II) by free chlorine and the presence of Mn(II) promote the formation of in situ Mn(II)-doped ferrihydrite. Kinetic modeling and characterization of Fe(III) oxides confirm that the heterogeneous catalytic effect of the Mn(II)-doped ferrihydrite, rather than manganese oxides or their coupled catalytic effect, is responsible for the enhanced oxidation rates. The doped Mn(II) substitutes the tetrahedral Fe(III) ions in the ferrihydrite, introducing additional negative charges at the doped sites. The increased charge enhances Mn(II) adsorption and lowers its redox potential, thereby accelerating Mn(II) oxidation rate through direct electron transfer with adjacent free chlorine. Additionally, the lepidocrocite formed by the reaction between Fe(II) and dissolved oxygen significantly impedes the catalytic performance. These findings provide new insights into the catalytic co-oxidation mechanism of Fe(II) and Mn(II), and help the optimization of water treatment engineering practices.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436331","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anaerobic fermentation combined with thermophilic bacteria (TB) pretreatment is a promising method to realize effective waste management and carbon resource recovery. However, undesirable properties of high-strength mariculture solid wastes (MSW) such as high solids concentration, excessive salinity and poor bioavailability limited the overall solubilization and acidogenic efficiency. This study innovatively introduced rhamnolipid (RL) to alleviate this adverse effect, and unveiled its cooperation with TB on enhancing organic matter dissolution and volatile fatty acids (VFAs) production. The results showed that VFAs yield from pretreated MSW was improved by 9.4-15.1 folds with enriched acetate (81.4%-94.4%) in the TB+RL groups. The co-pretreatment of RL and TB disintegrated substrate structure for efficient release of electron shuttles and biodegradable organics. This was because introducing RL reconstructed solid-liquid interfacial charge and molecular arrangement, improved thermophilic enzyme activity, and reduced apoptosis and necrosis cells of TB. Substrate bioavailability was further improved with proteinic structure shifted from α-helix and β-sheet to random coil and aggregated strands, and amide II and carboxyl groups interacted with RL molecules. These changes induced the selective enrichment of hydrolytic and acidogenic bacteria, and the upregulated expression of encoding genes responsible for transmembrane transport, protein hydrolysis, carbohydrate metabolism and acetate biosynthesis. This study provides a new strategy to overcome the bottlenecks of acidogenesis from high-strengthen organic wastes and deciphers the underlying mechanism.
{"title":"Cooperation of rhamnolipid and thermophilic bacteria modifies proteinic structure, microbial community, and metabolic traits for efficient solubilization and acidogenesis of mariculture solid wastes","authors":"Hutao Wang, Dongxu Xing, Chunji Jin, Yangguo Zhao, Liang Guo","doi":"10.1016/j.watres.2024.122634","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122634","url":null,"abstract":"Anaerobic fermentation combined with thermophilic bacteria (TB) pretreatment is a promising method to realize effective waste management and carbon resource recovery. However, undesirable properties of high-strength mariculture solid wastes (MSW) such as high solids concentration, excessive salinity and poor bioavailability limited the overall solubilization and acidogenic efficiency. This study innovatively introduced rhamnolipid (RL) to alleviate this adverse effect, and unveiled its cooperation with TB on enhancing organic matter dissolution and volatile fatty acids (VFAs) production. The results showed that VFAs yield from pretreated MSW was improved by 9.4-15.1 folds with enriched acetate (81.4%-94.4%) in the TB+RL groups. The co-pretreatment of RL and TB disintegrated substrate structure for efficient release of electron shuttles and biodegradable organics. This was because introducing RL reconstructed solid-liquid interfacial charge and molecular arrangement, improved thermophilic enzyme activity, and reduced apoptosis and necrosis cells of TB. Substrate bioavailability was further improved with proteinic structure shifted from α-helix and β-sheet to random coil and aggregated strands, and amide II and carboxyl groups interacted with RL molecules. These changes induced the selective enrichment of hydrolytic and acidogenic bacteria, and the upregulated expression of encoding genes responsible for transmembrane transport, protein hydrolysis, carbohydrate metabolism and acetate biosynthesis. This study provides a new strategy to overcome the bottlenecks of acidogenesis from high-strengthen organic wastes and deciphers the underlying mechanism.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-15DOI: 10.1016/j.watres.2024.122628
Baodan Jin, Ye Liu, Fukun Zhao, Yeyu Yan, Zhixuan Bai, Jingjing Du, Yuanqian Xu, Chuang Ma, Jiantao Ji
The effective production of NO2−-N through endogenous partial denitrification (EPD) provides a promising perspective for the broader adoption and application of anaerobic ammonia oxidation. However, the accumulation of polycyclic aromatic hydrocarbons (PAHs) in the environment may worsen the operational challenges of the EPD system. This study evaluated the resilience of the EPD system to the toxic impacts of phenanthrene (PHE) and anthracene (ANT) through macrogenomic analysis. A control group was maintained under identical conditions for comparison. The results revealed that PHE and ANT had a relatively minimal impact on NO3−-N transformation and organic matter removal but significantly affected PO43−-P removal and NO2−-N accumulation in the EPD process. The PHE system achieved a higher NO2−-N accumulation, with a maximum NO3−-N to NO2−-N conversion ratio of 90.08%. In contrast, the ANT system exhibited higher efficiency in the PO43−-P removal, achieving a peak removal rate of 74.94%. Macrogenomic analysis revealed that PAHs significantly enriched both denitrifying glycogen-accumulating organisms (including Candidatus_Competibacter) and denitrifying polyphosphate-accumulating organisms (such as Thauera, Candidatus_Contendobacter, and Candidatus_Accumulibacter). This enrichment stabilized these organisms, facilitating NO2−-N accumulation and PO43−-P removal. Metabolic pathway analysis indicated that PHE promoted the enrichment of NO3−-N reductase and inhibited NO2−-N reductase activity. However, ANT stimulated oxidative phosphorylation and the phosphate cycle. Moreover, PAH metabolites enhanced the expression of key genes encoding succinate dehydrogenase and isocitrate dehydrogenase in the tricarboxylic acid cycle within the EPD process, leading to increase the synthesis and utilization of acetyl coenzyme-A. Notably, significant differences were observed between the effects of PHE and ANT on these metabolic processes. This study provides new methods for treating PAH-containing wastewater through the combination of EPD and anaerobic ammonia oxidation.
{"title":"Macrogenomic analysis of tolerance and degradation mechanisms of polycyclic aromatic hydrocarbon in carbon and nitrogen metabolic pathways and associated bacterial communities during endogenous partial denitrification","authors":"Baodan Jin, Ye Liu, Fukun Zhao, Yeyu Yan, Zhixuan Bai, Jingjing Du, Yuanqian Xu, Chuang Ma, Jiantao Ji","doi":"10.1016/j.watres.2024.122628","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122628","url":null,"abstract":"The effective production of NO<sub>2</sub><sup>−</sup>-N through endogenous partial denitrification (EPD) provides a promising perspective for the broader adoption and application of anaerobic ammonia oxidation. However, the accumulation of polycyclic aromatic hydrocarbons (PAHs) in the environment may worsen the operational challenges of the EPD system. This study evaluated the resilience of the EPD system to the toxic impacts of phenanthrene (PHE) and anthracene (ANT) through macrogenomic analysis. A control group was maintained under identical conditions for comparison. The results revealed that PHE and ANT had a relatively minimal impact on NO<sub>3</sub><sup>−</sup>-N transformation and organic matter removal but significantly affected PO<sub>4</sub><sup>3−</sup>-P removal and NO<sub>2</sub><sup>−</sup>-N accumulation in the EPD process. The PHE system achieved a higher NO<sub>2</sub><sup>−</sup>-N accumulation, with a maximum NO<sub>3</sub><sup>−</sup>-N to NO<sub>2</sub><sup>−</sup>-N conversion ratio of 90.08%. In contrast, the ANT system exhibited higher efficiency in the PO<sub>4</sub><sup>3−</sup>-P removal, achieving a peak removal rate of 74.94%. Macrogenomic analysis revealed that PAHs significantly enriched both denitrifying glycogen-accumulating organisms (including <em>Candidatus_Competibacter</em>) and denitrifying polyphosphate-accumulating organisms (such as <em>Thauera, Candidatus_Contendobacter, and Candidatus_Accumulibacter</em>). This enrichment stabilized these organisms, facilitating NO<sub>2</sub><sup>−</sup>-N accumulation and PO<sub>4</sub><sup>3−</sup>-P removal. Metabolic pathway analysis indicated that PHE promoted the enrichment of NO<sub>3</sub><sup>−</sup>-N reductase and inhibited NO<sub>2</sub><sup>−</sup>-N reductase activity. However, ANT stimulated oxidative phosphorylation and the phosphate cycle. Moreover, PAH metabolites enhanced the expression of key genes encoding succinate dehydrogenase and isocitrate dehydrogenase in the tricarboxylic acid cycle within the EPD process, leading to increase the synthesis and utilization of acetyl coenzyme-A. Notably, significant differences were observed between the effects of PHE and ANT on these metabolic processes. This study provides new methods for treating PAH-containing wastewater through the combination of EPD and anaerobic ammonia oxidation.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439407","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-15DOI: 10.1016/j.watres.2024.122633
Jorge Salgado, Camila Jaramillo-Monroy, Andrés Link, Laura Lopera, Maria I. Velez, Catalina Gonzalez-Arango, Handong Yang, Virginia N. Panizzo, Suzanne McGowan
Tropical floodplain lakes are increasingly impacted by human activities, yet their pathways of spatial and temporal degradation, particularly under varying hydrological connectivity regimes and climate change, remain poorly understood. This study examines surface-sediment samples and 210Pb-dated sediment cores from six floodplain lakes, representing a gradient in hydrological connectivity in the lower Magdalena River Basin, Colombia. We analysed temporal and spatial variations in several sediment biogeochemical indicators: the concentration and flux of nutrients, heavy metals, and organic matter (OM), and redox conditions, flooding and erosion. Multiple factor analysis (MFA) of surface-sediments identified redox conditions, OM, flooding, heavy metals and lake connectivity as the main contributors to spatial variability within- and between-lakes sediments, accounting for 48% of the total variation. Additionally, no clear distinction was found between littoral and open-water sediment characteristics. Isolated lakes sediments exhibited reductive conditions rich in OM and nutrients, whereas connected lakes sediments showed greater heavy metal enrichment and higher concentrations of coarse river-fed material. Generalised additive models identified significant changes in the biogeochemical indicators since the late 1800s, that accelerated post-1980s. Shifts in OM, erosion, flooding, redox conditions, land-cover change, heavy metals and climate were identified by MFA as the main drivers of change, explaining 60%-71% of the variation in the connected lakes and 53%-72% in the isolated lakes. Post-1980s, connected lakes transitioned from conditions of higher accumulation of OM and little erosion to higher accumulation of heavy metals and river-fed material. Conversely, isolated lakes, shifted from detrital-heavy metal-rich sediments to OM-, and nutrient-rich, reductive sediments. Sedimentation rates also surged post-1980s, particularly in highly connected lakes, from 0.14 ± 0.07 g cm² yr⁻¹ to 0.5 ± 0.5 g cm² yr⁻¹, with elevated fluxes of metals, OM and nutrients. These changes in sediment biogeochemistry align with deforestation, river regulation and prolonged dry periods, highlighting the complexities behind establishing reliable reference conditions for pollution assessments in large, human-impacted tropical river systems.
热带洪泛平原湖泊正日益受到人类活动的影响,但人们对其空间和时间退化的途径,尤其是在不同的水文连通性机制和气候变化条件下的退化途径,仍然知之甚少。本研究考察了哥伦比亚马格达莱纳河流域下游代表水文连通性梯度的六个洪泛平原湖泊的表层沉积物样本和 210Pb 时间沉积物岩心。我们分析了几种沉积物生物地球化学指标的时空变化:营养物质、重金属和有机物(OM)的浓度和通量,以及氧化还原条件、洪水和侵蚀。表层沉积物的多因素分析(MFA)发现,氧化还原条件、OM、洪水、重金属和湖泊连通性是造成湖内和湖间沉积物空间变化的主要因素,占总变化的 48%。此外,沿岸沉积物特征与开阔水域沉积物特征之间没有明显区别。孤立湖泊的沉积物表现出富含 OM 和营养物质的还原性条件,而相连湖泊的沉积物则表现出更高的重金属富集度和更高的河流馈入粗物质浓度。广义加性模型发现,自 19 世纪末以来,生物地球化学指标发生了显著变化,这种变化在 20 世纪 80 年代后加速。多元回归分析法认为,OM、侵蚀、洪水、氧化还原条件、土地覆盖变化、重金属和气候的变化是导致变化的主要原因,可解释相连湖泊中 60%-71% 的变化,以及孤立湖泊中 53%-72% 的变化。20 世纪 80 年代后,相连湖泊从较高的 OM 积累和较少的侵蚀条件过渡到较高的重金属积累和河流饵料条件。与此相反,孤立湖泊则从富含碎屑重金属的沉积物转变为富含 OM 和营养物质的还原性沉积物。20 世纪 80 年代后,沉积速率也急剧上升,尤其是在高度连通的湖泊中,从 0.14 ± 0.07 g cm² yr-¹ 上升到 0.5 ± 0.5 g cm² yr-¹,金属、OM 和营养物质的通量也随之增加。沉积物生物地球化学的这些变化与森林砍伐、河流调节和长期干旱有关,凸显了在受人类影响的大型热带河流系统中建立可靠的污染评估参考条件的复杂性。
{"title":"Riverine connectivity modulates elemental fluxes through a 200- year period of intensive anthropic change in the Magdalena River floodplains, Colombia","authors":"Jorge Salgado, Camila Jaramillo-Monroy, Andrés Link, Laura Lopera, Maria I. Velez, Catalina Gonzalez-Arango, Handong Yang, Virginia N. Panizzo, Suzanne McGowan","doi":"10.1016/j.watres.2024.122633","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122633","url":null,"abstract":"Tropical floodplain lakes are increasingly impacted by human activities, yet their pathways of spatial and temporal degradation, particularly under varying hydrological connectivity regimes and climate change, remain poorly understood. This study examines surface-sediment samples and <sup>210</sup>Pb-dated sediment cores from six floodplain lakes, representing a gradient in hydrological connectivity in the lower Magdalena River Basin, Colombia. We analysed temporal and spatial variations in several sediment biogeochemical indicators: the concentration and flux of nutrients, heavy metals, and organic matter (OM), and redox conditions, flooding and erosion. Multiple factor analysis (MFA) of surface-sediments identified redox conditions, OM, flooding, heavy metals and lake connectivity as the main contributors to spatial variability within- and between-lakes sediments, accounting for 48% of the total variation. Additionally, no clear distinction was found between littoral and open-water sediment characteristics. Isolated lakes sediments exhibited reductive conditions rich in OM and nutrients, whereas connected lakes sediments showed greater heavy metal enrichment and higher concentrations of coarse river-fed material. Generalised additive models identified significant changes in the biogeochemical indicators since the late 1800s, that accelerated post-1980s. Shifts in OM, erosion, flooding, redox conditions, land-cover change, heavy metals and climate were identified by MFA as the main drivers of change, explaining 60%-71% of the variation in the connected lakes and 53%-72% in the isolated lakes. Post-1980s, connected lakes transitioned from conditions of higher accumulation of OM and little erosion to higher accumulation of heavy metals and river-fed material. Conversely, isolated lakes, shifted from detrital-heavy metal-rich sediments to OM-, and nutrient-rich, reductive sediments. Sedimentation rates also surged post-1980s, particularly in highly connected lakes, from 0.14 ± 0.07 g cm² yr⁻¹ to 0.5 ± 0.5 g cm² yr⁻¹, with elevated fluxes of metals, OM and nutrients. These changes in sediment biogeochemistry align with deforestation, river regulation and prolonged dry periods, highlighting the complexities behind establishing reliable reference conditions for pollution assessments in large, human-impacted tropical river systems.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436330","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dissolved organic matter (DOM) is a complex mixture that plays a crucial role in global carbon cycling and climate dynamics. Understanding the chemical composition of DOM is crucial for studying its biogeochemical behavior. However, identifying individual DOM molecules is challenging. Here, using ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry and an in-house database, we developed a framework to investigate DOM characteristics in natural water. Through the developed approach, we successfully identified thousands of individual DOM molecules in the water bodies of the Yangtze River Basin. For the first time, the proportions of natural and anthropogenic organics within DOM were revealed. In total, 9557 unambiguous molecular formulas were assigned to DOM in the Yangtze River Basin. The proportions of CHNO and CHOS compounds increased from upstream to downstream regions. Moreover, 1099 DOM compounds were tentatively identified, with 85% being endogenous organics and 15% being exogenous organics. Notably, lipids and pharmaceuticals and personal care products were the most frequently detected endogenous and exogenous compounds. The spatial variation of the identified DOM indicated anthropogenic discharges considerably increased both the number and abundance of DOM in the downstream Yangtze River Basin. This study highlighted the importance of anthropogenic impacts on DOM in water.
溶解有机物(DOM)是一种复杂的混合物,在全球碳循环和气候动力学中发挥着至关重要的作用。了解 DOM 的化学成分对研究其生物地球化学行为至关重要。然而,识别单个 DOM 分子具有挑战性。在此,我们利用超高分辨率傅立叶变换离子回旋共振质谱仪和内部数据库,开发了一种研究天然水中 DOM 特征的框架。通过所开发的方法,我们成功鉴定了长江流域水体中成千上万个独立的 DOM 分子。首次揭示了 DOM 中天然有机物和人为有机物的比例。共为长江流域的 DOM 分配了 9557 个明确的分子式。从上游到下游,CHNO 和 CHOS 化合物的比例有所增加。此外,还初步鉴定出 1099 种 DOM 化合物,其中 85% 为内源有机物,15% 为外源有机物。值得注意的是,脂类和药物及个人护理产品是最常检测到的内源和外源化合物。已鉴定 DOM 的空间变化表明,人为排放大大增加了长江下游流域 DOM 的数量和丰度。这项研究强调了人为因素对水中 DOM 影响的重要性。
{"title":"Characterization of Natural and Anthropogenic Dissolved Organic Matter in the Yangtze River Basin Using FT-ICR MS","authors":"Cuiping Ning, Shuai Sun, Yuan Gao, Huaijun Xie, Lidong Wu, Haijun Zhang, Jiping Chen, Ningbo Geng","doi":"10.1016/j.watres.2024.122636","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122636","url":null,"abstract":"Dissolved organic matter (DOM) is a complex mixture that plays a crucial role in global carbon cycling and climate dynamics. Understanding the chemical composition of DOM is crucial for studying its biogeochemical behavior. However, identifying individual DOM molecules is challenging. Here, using ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry and an in-house database, we developed a framework to investigate DOM characteristics in natural water. Through the developed approach, we successfully identified thousands of individual DOM molecules in the water bodies of the Yangtze River Basin. For the first time, the proportions of natural and anthropogenic organics within DOM were revealed. In total, 9557 unambiguous molecular formulas were assigned to DOM in the Yangtze River Basin. The proportions of CHNO and CHOS compounds increased from upstream to downstream regions. Moreover, 1099 DOM compounds were tentatively identified, with 85% being endogenous organics and 15% being exogenous organics. Notably, lipids and pharmaceuticals and personal care products were the most frequently detected endogenous and exogenous compounds. The spatial variation of the identified DOM indicated anthropogenic discharges considerably increased both the number and abundance of DOM in the downstream Yangtze River Basin. This study highlighted the importance of anthropogenic impacts on DOM in water.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439920","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The application of Fe-catalyzed periodate (PI) processes is often limited by both the narrow applicable pH range and weak reaction between Fe(III) and oxidant. Here, the biodegradable picolinic acid (PICA) was used as one kind of chelating ligands (CLs) to enhance the removal of organic pollutants (OPs) at initial pH 3.0−8.0, which displayed superior properties than the other CLs in Fe(III)/PI process. The dominant reactive species produced in the Fe(III)-PICA/PI process turned out to be high-valent iron-oxo (FeIV=O) species and hydroxyl radical (•OH) by quenching, sulfoxide probe transformation, and 18O isotope-labeling tests. The relative contribution of FeIV=O and •OH was dependent on OPs ionization potential (IP) and energy gap (ΔE). The degradation of OPs was also directly associated with their structure, the apparent rate constants correlated well with the highest occupied molecular orbital energy (EHOMO), IP, and ΔE, and among them ΔE had a greater effect. Furthermore, Fe(III)-PICA complexes displayed excellent long-term effectiveness for OPs removal in actual water matrixes, along with the non-toxic conversion of PI, indicating a broad application perspective of Fe(III)-PICA/PI process. This study provides an efficient method to improve the performance of Fe(III)/PI process and reveals the mechanism and relationship between removal efficiency and pollutant structure.
{"title":"Picolinic acid promotes organic pollutants removal in Fe(III)/periodate process: Mechanism and relationship between removal efficiency and pollutant structure","authors":"Jiansen Lei, Linjie Ding, Yangju Li, Xiang Li, Siyuan Pan, Dapeng Wu, Kai Jiang","doi":"10.1016/j.watres.2024.122631","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122631","url":null,"abstract":"The application of Fe-catalyzed periodate (PI) processes is often limited by both the narrow applicable pH range and weak reaction between Fe(III) and oxidant. Here, the biodegradable picolinic acid (PICA) was used as one kind of chelating ligands (CLs) to enhance the removal of organic pollutants (OPs) at initial pH 3.0−8.0, which displayed superior properties than the other CLs in Fe(III)/PI process. The dominant reactive species produced in the Fe(III)-PICA/PI process turned out to be high-valent iron-oxo (Fe<sup>IV</sup>=O) species and hydroxyl radical (<sup>•</sup>OH) by quenching, sulfoxide probe transformation, and <sup>18</sup>O isotope-labeling tests. The relative contribution of Fe<sup>IV</sup>=O and <sup>•</sup>OH was dependent on OPs ionization potential (IP) and energy gap (ΔE). The degradation of OPs was also directly associated with their structure, the apparent rate constants correlated well with the highest occupied molecular orbital energy (E<sub>HOMO</sub>), IP, and ΔE, and among them ΔE had a greater effect. Furthermore, Fe(III)-PICA complexes displayed excellent long-term effectiveness for OPs removal in actual water matrixes, along with the non-toxic conversion of PI, indicating a broad application perspective of Fe(III)-PICA/PI process. This study provides an efficient method to improve the performance of Fe(III)/PI process and reveals the mechanism and relationship between removal efficiency and pollutant structure.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436332","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-13DOI: 10.1016/j.watres.2024.122627
Jiahao Sun, Minjia Yan, Guangdong Tao, Runbin Su, Xuanming Xiao, Qiangshun Wu, Feng Chen, Xi-Lin Wu, Hongjun Lin
Single-atom nanozymes possess high catalytic activity and selectivity, and are emerging as advanced heterogeneous catalysts for environmental applications. Herein, we present the innovative synthesis and characterization of a single-atom manganese-doped carbon nitride (SA-Mn-CN) nanozyme, integrated into a polyvinylidene fluoride (PVDF) membrane for advanced water treatment applications. The SA-Mn-CN nanozyme demonstrates high peroxidase-like activity, efficiently catalyzing the oxidation of 3,3’,5,5’-tetramethylbenzidine (TMB) and generating reactive oxygen species (ROS) for effective antibacterial action. Notably, the SA-Mn-CN/PVDF membrane showcases enhanced water permeability, superior antifouling properties, and ultra-fast degradation kinetics of organic pollutants. Mechanistic studies reveal that the nanozyme selectively generates Mn(IV)-oxo species via peroxymonosulfate (PMS) activation, crucial for the efficient oxidation processes. Our integrated membrane system effectively removes (within 1 min, > 92% removal) a variety of organic micropollutants in continuous-flow operations, demonstrating excellent stability and minimal manganese leaching. Compared to conventional advanced oxidation process (AOPs)/membrane system, the SA-Mn-CN/PVDF/PMS system holds the advantages of high catalytic activity and selectivity for generation of reactive species, wide working pH range (pH3-11) and excellent stability and reusability under the backwashing conditions. The developed device-scale AOPs/membrane system was proven to be effective in bacterial inactivation and pollutants degradation, verifying the vast application potential of the SA-Mn-CN/PVDF membrane for practical water decontamination. This work pioneers the development of enzyme-mimicking nanozyme membranes, offering a sustainable and high-performance solution for wastewater treatment, and sets a new benchmark for the design of nanozyme-based catalytic membranes in environmental applications.
{"title":"A single-atom manganese nanozyme mediated membrane reactor for water decontamination","authors":"Jiahao Sun, Minjia Yan, Guangdong Tao, Runbin Su, Xuanming Xiao, Qiangshun Wu, Feng Chen, Xi-Lin Wu, Hongjun Lin","doi":"10.1016/j.watres.2024.122627","DOIUrl":"https://doi.org/10.1016/j.watres.2024.122627","url":null,"abstract":"Single-atom nanozymes possess high catalytic activity and selectivity, and are emerging as advanced heterogeneous catalysts for environmental applications. Herein, we present the innovative synthesis and characterization of a single-atom manganese-doped carbon nitride (SA-Mn-CN) nanozyme, integrated into a polyvinylidene fluoride (PVDF) membrane for advanced water treatment applications. The SA-Mn-CN nanozyme demonstrates high peroxidase-like activity, efficiently catalyzing the oxidation of 3,3’,5,5’-tetramethylbenzidine (TMB) and generating reactive oxygen species (ROS) for effective antibacterial action. Notably, the SA-Mn-CN/PVDF membrane showcases enhanced water permeability, superior antifouling properties, and ultra-fast degradation kinetics of organic pollutants. Mechanistic studies reveal that the nanozyme selectively generates Mn(IV)-oxo species via peroxymonosulfate (PMS) activation, crucial for the efficient oxidation processes. Our integrated membrane system effectively removes (within 1 min, > 92% removal) a variety of organic micropollutants in continuous-flow operations, demonstrating excellent stability and minimal manganese leaching. Compared to conventional advanced oxidation process (AOPs)/membrane system, the SA-Mn-CN/PVDF/PMS system holds the advantages of high catalytic activity and selectivity for generation of reactive species, wide working pH range (pH3-11) and excellent stability and reusability under the backwashing conditions. The developed device-scale AOPs/membrane system was proven to be effective in bacterial inactivation and pollutants degradation, verifying the vast application potential of the SA-Mn-CN/PVDF membrane for practical water decontamination. This work pioneers the development of enzyme-mimicking nanozyme membranes, offering a sustainable and high-performance solution for wastewater treatment, and sets a new benchmark for the design of nanozyme-based catalytic membranes in environmental applications.","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":12.8,"publicationDate":"2024-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142431696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}