首页 > 最新文献

Water Research最新文献

英文 中文
Prioritizing conservation sites for multi-pond systems to maintain protection of water quality in a fragmented agricultural catchment 为多池塘系统确定保护地点的优先次序,以保持对支离破碎的农业集水区水质的保护
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-07 DOI: 10.1016/j.watres.2024.122763
Haozhe Zhang , Yuhai Bao , Xiubin He , Jiaorong Lv , Qiang Tang , Xiaomin Qin , Adrian L. Collins
Precise targeting of conservation practices to the most effective sites in multi-pond systems (MPSs) is critical for resource optimization and water quality improvement. Previous studies generally prioritized ponds for conservation practices considering nutrient removal efficiency. However, they have frequently overlooked the role of ponds in sediment interception and the impact of human activities and environmental factors around the pond. Herein, the present study developed and applied a novel framework for pond prioritization by integrating the Pressure-State-Response (PSR) model, graph theory, and K-mean clustering. The framework consists of three components. An indicator system is developed to represent the nutrient removal performance of any MPS, impacts on catchment sediment connectivity, external threats, and human-initiated conservation. A flow path network considering natural and artificial elements was constructed to calculate indicator values. A cluster analysis was conducted on the index values of different ponds, and a hierarchical sorting method were used to prioritize ponds. The framework was applied to the Guilinqiao Catchment, a typical fragmented agricultural catchment in the Yangtze River Basin, China. The study has quantified the Pressure, State, and Response indices of different ponds in this catchment, prioritized the ponds, and drawn recommendations for conserving MPSs based on field surveys and remote sensing data. Ponds with higher Pressure index, higher State index, and lower Response index scores should be targeted as conservation priorities. This framework provides an effective method for ensuring management of MPSs to sustainably maximize water cleanup capacity with limited resources.
在多池塘系统(MPS)中,将保护措施精确定位到最有效的地点对于资源优化和水质改善至关重要。以往的研究通常会考虑养分去除效率,优先选择池塘进行保护实践。然而,这些研究往往忽略了池塘在拦截沉积物方面的作用以及池塘周围人类活动和环境因素的影响。在此,本研究通过整合压力-状态-响应(PSR)模型、图论和 K-均值聚类,开发并应用了一种新的池塘优先排序框架。该框架由三部分组成。开发了一个指标体系,用于表示任何 MPS 的营养物去除性能、对集水区沉积物连通性的影响、外部威胁以及人类发起的保护。为计算指标值,构建了一个考虑自然和人工要素的流路网络。对不同池塘的指标值进行聚类分析,并采用分层排序法对池塘进行优先排序。该框架应用于桂林桥流域,这是中国长江流域典型的碎片化农业集水区。研究基于实地调查和遥感数据,量化了该流域不同池塘的压力指数、状态指数和响应指数,确定了池塘的优先次序,并提出了保护多源保护区的建议。压力指数较高、状态指数较高和响应指数较低的池塘应作为优先保护对象。该框架提供了一种有效的方法,可确保对多水层保护区进行管理,从而在资源有限的情况下可持续地最大限度提高水体净化能力。
{"title":"Prioritizing conservation sites for multi-pond systems to maintain protection of water quality in a fragmented agricultural catchment","authors":"Haozhe Zhang ,&nbsp;Yuhai Bao ,&nbsp;Xiubin He ,&nbsp;Jiaorong Lv ,&nbsp;Qiang Tang ,&nbsp;Xiaomin Qin ,&nbsp;Adrian L. Collins","doi":"10.1016/j.watres.2024.122763","DOIUrl":"10.1016/j.watres.2024.122763","url":null,"abstract":"<div><div>Precise targeting of conservation practices to the most effective sites in multi-pond systems (MPSs) is critical for resource optimization and water quality improvement. Previous studies generally prioritized ponds for conservation practices considering nutrient removal efficiency. However, they have frequently overlooked the role of ponds in sediment interception and the impact of human activities and environmental factors around the pond. Herein, the present study developed and applied a novel framework for pond prioritization by integrating the Pressure-State-Response (PSR) model, graph theory, and K-mean clustering. The framework consists of three components. An indicator system is developed to represent the nutrient removal performance of any MPS, impacts on catchment sediment connectivity, external threats, and human-initiated conservation. A flow path network considering natural and artificial elements was constructed to calculate indicator values. A cluster analysis was conducted on the index values of different ponds, and a hierarchical sorting method were used to prioritize ponds. The framework was applied to the Guilinqiao Catchment, a typical fragmented agricultural catchment in the Yangtze River Basin, China. The study has quantified the Pressure, State, and Response indices of different ponds in this catchment, prioritized the ponds, and drawn recommendations for conserving MPSs based on field surveys and remote sensing data. Ponds with higher Pressure index, higher State index, and lower Response index scores should be targeted as conservation priorities. This framework provides an effective method for ensuring management of MPSs to sustainably maximize water cleanup capacity with limited resources.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122763"},"PeriodicalIF":11.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594446","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}
引用次数: 0
Long-term effects of dead algal deposition on sediment surfaces: Behavior of endogenous phosphorus release in sediments 死藻沉积对沉积物表面的长期影响:沉积物中的内源磷释放行为
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-06 DOI: 10.1016/j.watres.2024.122742
Yanqi Chen , Dapeng Li , Songqi Liu , Yujie Zhang , Xinrui Yan , Xinyu Song , Ziyu Li , Boling Li , Sujie Shan , Yizhi Zhu , Jun Hou
Algae blooms are frequently triggered owing to the improvements in aquatic trophic levels. The aggregated algae from these blooms are eventually dead and accumulate on sediment surfaces, impacting the microenvironment and phosphorus cycling in aquatic systems. However, research on the effects of naturally dead algal deposition on endogenous P release from sediments is lacking. In this study, we investigated the long-term effects of dead algal deposition at varying concentrations on P release from sediments and the underlying mechanisms by assessing microbial metabolism and community structure. The results showed that following the dead algal deposition, the release of P from sediments to the water column peaked on day 40 (0.14±0.017 mg L-1 in Amend12) and the SRP exchange capacity reached maximum (6.09 ± 1.63 mg/(cm2·d) in Amend12) at sediment-water interface in phase1 (0–3 day). This might be primarily attributed to the deposition of dead algae introducing much organic matter (such as organic carbon and organic phosphorus), thus altering the sediment microenvironment, which increased the activity of phosphorus-cycle microorganisms, such as polyphosphate-accumulating organisms, through increasing C source metabolism, reducing intracellular ammonia inhibition, and creating more suitable anaerobic conditions. Therefore, this study has improved our understanding of the management strategies for controlling endogenous phosphorus release in eutrophic shallow lakes, suggesting that the priming effects of freshly deposited algae could be mitigated by harvesting algae at the peak of blooms.
水生营养级的提高经常会引发藻华。藻华产生的聚集藻类最终会死亡,并堆积在沉积物表面,影响水生系统的微环境和磷循环。然而,有关自然死亡藻类沉积对沉积物内源磷释放的影响的研究还很缺乏。在这项研究中,我们通过评估微生物代谢和群落结构,研究了不同浓度的死藻沉积对沉积物中磷释放的长期影响及其内在机制。结果表明,死藻沉积后,沉积物向水体的 P 释放量在第 40 天达到峰值(Amend12 为 0.14±0.017 mg L-1),SRP 交换能力在第一阶段(0-3 天)达到最大值(Amend12 为 6.09±1.63 mg/(cm2-d))。这可能主要归因于死亡藻类的沉积引入了大量的有机质(如有机碳和有机磷),从而改变了沉积物的微环境,通过增加C源代谢、减少细胞内氨抑制和创造更合适的厌氧条件,提高了磷循环微生物(如聚磷酸盐积累生物)的活性。因此,这项研究加深了我们对控制富营养化浅水湖泊内源磷释放的管理策略的理解,表明在藻类繁殖高峰期收割藻类可减轻新沉积藻类的引诱效应。
{"title":"Long-term effects of dead algal deposition on sediment surfaces: Behavior of endogenous phosphorus release in sediments","authors":"Yanqi Chen ,&nbsp;Dapeng Li ,&nbsp;Songqi Liu ,&nbsp;Yujie Zhang ,&nbsp;Xinrui Yan ,&nbsp;Xinyu Song ,&nbsp;Ziyu Li ,&nbsp;Boling Li ,&nbsp;Sujie Shan ,&nbsp;Yizhi Zhu ,&nbsp;Jun Hou","doi":"10.1016/j.watres.2024.122742","DOIUrl":"10.1016/j.watres.2024.122742","url":null,"abstract":"<div><div>Algae blooms are frequently triggered owing to the improvements in aquatic trophic levels. The aggregated algae from these blooms are eventually dead and accumulate on sediment surfaces, impacting the microenvironment and phosphorus cycling in aquatic systems. However, research on the effects of naturally dead algal deposition on endogenous P release from sediments is lacking. In this study, we investigated the long-term effects of dead algal deposition at varying concentrations on P release from sediments and the underlying mechanisms by assessing microbial metabolism and community structure. The results showed that following the dead algal deposition, the release of P from sediments to the water column peaked on day 40 (0.14±0.017 mg L<sup>-1</sup> in Amend12) and the SRP exchange capacity reached maximum (6.09 ± 1.63 mg/(cm<sup>2</sup>·d) in Amend12) at sediment-water interface in phase1 (0–3 day). This might be primarily attributed to the deposition of dead algae introducing much organic matter (such as organic carbon and organic phosphorus), thus altering the sediment microenvironment, which increased the activity of phosphorus-cycle microorganisms, such as polyphosphate-accumulating organisms, through increasing C source metabolism, reducing intracellular ammonia inhibition, and creating more suitable anaerobic conditions. Therefore, this study has improved our understanding of the management strategies for controlling endogenous phosphorus release in eutrophic shallow lakes, suggesting that the priming effects of freshly deposited algae could be mitigated by harvesting algae at the peak of blooms.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122742"},"PeriodicalIF":11.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594479","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}
引用次数: 0
Nano-micro materials regulated biocatalytic metabolism for efficient environmental remediation: Fine engineering the mass and electron transfer in multicellular environments 纳米微材料调节生物催化新陈代谢,实现高效环境修复:多细胞环境中质量和电子转移的精细工程设计
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-06 DOI: 10.1016/j.watres.2024.122759
Haojin Peng, Yu Su, Xinyun Fan, Shuai Wang, Qingran Zhang, Yinguang Chen
The escalating energy and environmental crises have spurred significant research interest into developing efficient biological remediation technologies for sustainable contaminant and resource conversion. Integrating engineered nano-micro materials (NMMs) with these biocatalytic processes offers a promising approach to improve the microbial performance for environmental remediation. Core to such material-enhanced hybrid biocatalysis systems (MHBSs) is the rational regulation of metabolic processes with the assistance of NMMs, where a fine engineered mass and electron transfer is beneficial for the improved biocatalytic activity. However, the specific mechanisms of those NMMs-enhanced microbial metabolisms are normally overlooked. Here, we review the recent progress in MHBSs, focusing primarily on the mass/electron transfer regulation strategies for an enhanced microbial behavior. Specifically, the NMMs-regulated mass and electron transfer in extracellular, interfacial, and intracellular environment are summarized, where the patterns of diverse microbiological response are discussed thoroughly. Notably, fine modifications of cell interfaces and intracellular compartments by NMMs could even endow the biohybrids with new metabolic functions beyond their natural capabilities. Further, we also emphasize the importance of matching the various metabolic demands of biosystems with the diverse properties of NMMs to achieve efficient environmental remediation through a coordinated regulation strategy. Finally, major challenges and opportunities for the future development and practical implementation of MHBSs for environment remediation practices are given, aiming to provide future system design guidelines for attaining desirable biological behaviors.
不断升级的能源和环境危机激发了人们对开发可持续污染物和资源转化的高效生物修复技术的极大研究兴趣。将工程纳米微材料(NMMs)与这些生物催化过程相结合,为改善微生物的环境修复性能提供了一种前景广阔的方法。这种材料增强型混合生物催化系统(MHBSs)的核心是在 NMMs 的协助下合理调节代谢过程,其中精细设计的质量和电子转移有利于提高生物催化活性。然而,NMMs 增强微生物代谢的具体机制通常被忽视。在此,我们回顾了 MHBS 的最新进展,主要侧重于质量/电子传递调控策略,以增强微生物的行为。具体来说,我们总结了 NMMs 在细胞外、界面和细胞内环境中调控的质量和电子传递,并深入探讨了微生物的不同反应模式。值得注意的是,NMMs 对细胞界面和细胞内隔室的精细修饰甚至可以赋予生物杂交体新的代谢功能,超越其天然能力。此外,我们还强调了将生物系统的各种代谢需求与 NMM 的各种特性相匹配的重要性,以便通过协调的调节策略实现高效的环境修复。最后,我们给出了未来开发和实际应用 MHBSs 进行环境修复实践所面临的主要挑战和机遇,旨在为实现理想的生物行为提供未来的系统设计指南。
{"title":"Nano-micro materials regulated biocatalytic metabolism for efficient environmental remediation: Fine engineering the mass and electron transfer in multicellular environments","authors":"Haojin Peng,&nbsp;Yu Su,&nbsp;Xinyun Fan,&nbsp;Shuai Wang,&nbsp;Qingran Zhang,&nbsp;Yinguang Chen","doi":"10.1016/j.watres.2024.122759","DOIUrl":"10.1016/j.watres.2024.122759","url":null,"abstract":"<div><div>The escalating energy and environmental crises have spurred significant research interest into developing efficient biological remediation technologies for sustainable contaminant and resource conversion. Integrating engineered nano-micro materials (NMMs) with these biocatalytic processes offers a promising approach to improve the microbial performance for environmental remediation. Core to such material-enhanced hybrid biocatalysis systems (MHBSs) is the rational regulation of metabolic processes with the assistance of NMMs, where a fine engineered mass and electron transfer is beneficial for the improved biocatalytic activity. However, the specific mechanisms of those NMMs-enhanced microbial metabolisms are normally overlooked. Here, we review the recent progress in MHBSs, focusing primarily on the mass/electron transfer regulation strategies for an enhanced microbial behavior. Specifically, the NMMs-regulated mass and electron transfer in extracellular, interfacial, and intracellular environment are summarized, where the patterns of diverse microbiological response are discussed thoroughly. Notably, fine modifications of cell interfaces and intracellular compartments by NMMs could even endow the biohybrids with new metabolic functions beyond their natural capabilities. Further, we also emphasize the importance of matching the various metabolic demands of biosystems with the diverse properties of NMMs to achieve efficient environmental remediation through a coordinated regulation strategy. Finally, major challenges and opportunities for the future development and practical implementation of MHBSs for environment remediation practices are given, aiming to provide future system design guidelines for attaining desirable biological behaviors.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122759"},"PeriodicalIF":11.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589012","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}
引用次数: 0
Photoaging-induced variations in heteroaggregation of nanoplastics and suspended sediments in aquatic environments: A case study on nanopolystyrene 水生环境中纳米塑料和悬浮沉积物异质聚集的光照诱导变化:纳米聚苯乙烯案例研究
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-06 DOI: 10.1016/j.watres.2024.122762
Dan Luo , Chang Li , Xue Bai , Yi Shi , Ruifeng Wang
Photoaging of nanoplastics (NPs) and heteroaggregate with suspended sediments (SS) determines transport processes and ecological risks of NPs in aquatic environments. This study investigated the disruption of photoaging on the heteroaggregation behavior of polystyrene NPs (PSNPs) and SS in different valence electrolyte solutions and deduced the interaction mechanisms by integrating aggregation kinetics and molecular dynamics (MD) simulation. Increasing the electrolyte concentration significantly enhanced the heteroaggregation between PSNPs and SS, and the divalent electrolytes induced the heteroaggregation more efficiently. MD simulation at the molecular level revealed that PS and SS could spontaneously form clusters, and photoaged PS has a stronger potential to fold into a dense state with SS. Photoaging for 30 d retarded heteroaggregation due to the steric hindrance produced by the leached organic matter in NaCl solutions, and the critical coagulation concentration (CCC) increased by >85.44 %. Contrarily, photoaging caused more oxygen-containing functional groups produced on the surface of PSNPs through Ca2+ bridging promoting heteroaggregation and thus destabilizing in CaCl2 solutions, the CCC decreased by 23.53 % ∼ 35.29 %. These findings provide mechanistic insight into the environmental process of NPs and SS and are crucial for a comprehensive understanding of the environmental fate and transport of NPs in aquatic environments.
纳米塑料(NPs)的光老化和与悬浮沉积物(SS)的异质聚集决定了 NPs 在水生环境中的迁移过程和生态风险。本研究探讨了光老化对不同价态电解质溶液中聚苯乙烯 NPs(PSNPs)与悬浮物异质聚集行为的干扰,并结合聚集动力学和分子动力学(MD)模拟推导了其相互作用机理。电解质浓度的增加显著增强了聚苯乙烯纳米粒子和聚苯乙烯砜之间的异质聚集,二价电解质诱导异质聚集的效率更高。分子水平上的 MD 模拟显示,PS 和 SS 可自发形成团簇,光老化 PS 与 SS 折叠成致密状态的潜力更大。由于 NaCl 溶液中浸出有机物产生的立体阻碍作用,光照 30 d 可延缓异聚,临界凝结浓度(CCC)提高了 85.44% 以上。相反,在 CaCl2 溶液中,光aging 通过 Ca2+ 桥接作用使 PSNPs 表面产生更多含氧官能团,促进异聚,从而破坏稳定性,CCC 降低了 23.53% ∼ 35.29%。这些发现从机理上揭示了 NPs 和 SS 的环境过程,对于全面了解 NPs 在水生环境中的环境归宿和迁移至关重要。
{"title":"Photoaging-induced variations in heteroaggregation of nanoplastics and suspended sediments in aquatic environments: A case study on nanopolystyrene","authors":"Dan Luo ,&nbsp;Chang Li ,&nbsp;Xue Bai ,&nbsp;Yi Shi ,&nbsp;Ruifeng Wang","doi":"10.1016/j.watres.2024.122762","DOIUrl":"10.1016/j.watres.2024.122762","url":null,"abstract":"<div><div>Photoaging of nanoplastics (NPs) and heteroaggregate with suspended sediments (SS) determines transport processes and ecological risks of NPs in aquatic environments. This study investigated the disruption of photoaging on the heteroaggregation behavior of polystyrene NPs (PSNPs) and SS in different valence electrolyte solutions and deduced the interaction mechanisms by integrating aggregation kinetics and molecular dynamics (MD) simulation. Increasing the electrolyte concentration significantly enhanced the heteroaggregation between PSNPs and SS, and the divalent electrolytes induced the heteroaggregation more efficiently. MD simulation at the molecular level revealed that PS and SS could spontaneously form clusters, and photoaged PS has a stronger potential to fold into a dense state with SS. Photoaging for 30 d retarded heteroaggregation due to the steric hindrance produced by the leached organic matter in NaCl solutions, and the critical coagulation concentration (CCC) increased by &gt;85.44 %. Contrarily, photoaging caused more oxygen-containing functional groups produced on the surface of PSNPs through Ca<sup>2+</sup> bridging promoting heteroaggregation and thus destabilizing in CaCl<sub>2</sub> solutions, the CCC decreased by 23.53 % ∼ 35.29 %. These findings provide mechanistic insight into the environmental process of NPs and SS and are crucial for a comprehensive understanding of the environmental fate and transport of NPs in aquatic environments.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122762"},"PeriodicalIF":11.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594478","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}
引用次数: 0
Development of a deep learning–based feature stream network for forecasting riverine harmful algal blooms from a network perspective 从网络角度开发基于深度学习的特征流网络,用于预报河流有害藻华
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-05 DOI: 10.1016/j.watres.2024.122751
Jihoon Shin, YoonKyung Cha
Global increases in the occurrence of harmful algal blooms (HABs) are of major concern in water quality and resource management. A predictive model capable of quantifying the spatiotemporal associations between HABs and their influencing factors is required for effective preventive management. In this study, a feature stream network (FSN) model is proposed to provide daily forecasts of cyanobacteria abundance at multiple monitoring sites simultaneously in a river network. The spatial connectivity between monitoring sites was expressed as a directed acyclic graph comprising edges and nodes representing flows and monitoring sites, respectively. Furthermore, a segment-wise node connection structure was developed to extract the latent features of a river segment comprising individual nodes and sequentially transfer them to the downstream segment(s). In addition, a feature engineering–attention hybrid mechanism was employed to address temporal mismatches among different monitoring schemes while adding explainability to the model. Consequently, the FSN showed improved predictive performance, temporal resolution, and explainability for multi-site forecasts of HAB in a single model framework. The developed model was applied to a bloom-prone middle course of the Nakdong River, South Korea. Various hydrological, environmental, and biological factors were utilized for forecasting the cyanobacteria abundance. The FSN exhibited a high degree of accuracy across the sites for the test data with a coefficient of determination in the range of 0.64–0.71 and root mean square error in the range of 2.06–2.26 cells/mL on natural log scales. Although the relative importance of input features varied across the sites, the features extracted from nearby nodes consistently exhibited high importance in forecasting the cyanobacteria abundance. These explanations indicate that the proposed model can successfully characterize the spatial hierarchy of a river network. A scenario analysis suggested that reduced total nitrogen loads in the effluents from the wastewater treatment plant and the combined operations of upstream and downstream weirs were effective in managing HABs.
全球有害藻华(HABs)发生率的增加是水质和资源管理方面的一个重大问题。为了进行有效的预防管理,需要一个能够量化有害藻华及其影响因素之间时空关联的预测模型。本研究提出了一种特征流网络(FSN)模型,用于同时预测河网中多个监测点的蓝藻丰度。监测点之间的空间连通性用有向无环图表示,图中的边和节点分别代表流量和监测点。此外,还开发了分段节点连接结构,以提取由单个节点组成的河段的潜在特征,并依次将其转移到下游河段。此外,还采用了特征工程-关注混合机制,以解决不同监测方案之间的时间不匹配问题,同时增加模型的可解释性。因此,在单一模型框架内,FSN 在多站点预测 HAB 方面显示出更高的预测性能、时间分辨率和可解释性。所开发的模型被应用于韩国洛东江水华易发的中游河道。利用各种水文、环境和生物因素来预测蓝藻的丰度。在各站点的测试数据中,FSN 都表现出较高的准确性,其决定系数范围为 0.64-0.71,均方根误差范围为 2.06-2.26 cells/mL(自然对数)。尽管输入特征的相对重要性在不同地点有所不同,但从附近节点提取的特征在预测蓝藻丰度时始终表现出较高的重要性。这些说明所提出的模型可以成功地描述河网的空间层次结构。情景分析表明,减少污水处理厂排放物中的总氮负荷以及上下游围堰的联合运行可有效治理 HABs。
{"title":"Development of a deep learning–based feature stream network for forecasting riverine harmful algal blooms from a network perspective","authors":"Jihoon Shin,&nbsp;YoonKyung Cha","doi":"10.1016/j.watres.2024.122751","DOIUrl":"10.1016/j.watres.2024.122751","url":null,"abstract":"<div><div>Global increases in the occurrence of harmful algal blooms (HABs) are of major concern in water quality and resource management. A predictive model capable of quantifying the spatiotemporal associations between HABs and their influencing factors is required for effective preventive management. In this study, a feature stream network (FSN) model is proposed to provide daily forecasts of cyanobacteria abundance at multiple monitoring sites simultaneously in a river network. The spatial connectivity between monitoring sites was expressed as a directed acyclic graph comprising edges and nodes representing flows and monitoring sites, respectively. Furthermore, a segment-wise node connection structure was developed to extract the latent features of a river segment comprising individual nodes and sequentially transfer them to the downstream segment(s). In addition, a feature engineering–attention hybrid mechanism was employed to address temporal mismatches among different monitoring schemes while adding explainability to the model. Consequently, the FSN showed improved predictive performance, temporal resolution, and explainability for multi-site forecasts of HAB in a single model framework. The developed model was applied to a bloom-prone middle course of the Nakdong River, South Korea. Various hydrological, environmental, and biological factors were utilized for forecasting the cyanobacteria abundance. The FSN exhibited a high degree of accuracy across the sites for the test data with a coefficient of determination in the range of 0.64–0.71 and root mean square error in the range of 2.06–2.26 cells/mL on natural log scales. Although the relative importance of input features varied across the sites, the features extracted from nearby nodes consistently exhibited high importance in forecasting the cyanobacteria abundance. These explanations indicate that the proposed model can successfully characterize the spatial hierarchy of a river network. A scenario analysis suggested that reduced total nitrogen loads in the effluents from the wastewater treatment plant and the combined operations of upstream and downstream weirs were effective in managing HABs.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122751"},"PeriodicalIF":11.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142579838","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}
引用次数: 0
Reconsideration of the role of hydrogen peroxide in peroxymonocarbonate-based oxidation system for pollutant control 重新考虑过氧化氢在基于过氧一碳酸盐的污染物控制氧化系统中的作用
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-05 DOI: 10.1016/j.watres.2024.122750
Zihan Yang , Yi Zhou , Yiqian Jiang , Peiqing Zhao , Xu Meng
Advanced oxidation processes that utilize peroxymonocarbonate (HCO4-), generated in-situ through the reaction of HCO3- and H2O2, are employed for the removal of pollutants in water. Nevertheless, the precise role of H2O2 in these processes remains a subject of debate. This study established a HCO4--based oxidation system using NaHCO3 and H2O2 for the degradation of acetaminophen and investigated the activation mechanisms of coexisting oxidants. Under thermal activation conditions, the OO bond in HCO4- (HOOCOO-) was more readily cleaved than the OO bond in the co-existing oxidant H2O2 (HOOH), leading to the generation of reactive oxygen species (ROS). Based on kinetics and ROS evaluation, H2O2 primarily served to form HCO4- rather than converting to ·OH or O2, with HCO4- acting as the primary oxidant for degradation through the formation of CO3·and ·OH. In this oxidation system, H2O2 utilization efficiency for ·OH production reached 27.34 %, ·OH yield reached 24.15 % and acetaminophen degradation efficiency realized 83 % at 60 °C with 20 mM HCO3- and 20 mM H2O2. The apparent activation energy of acetaminophen degradation and HCO4- activation were calculated as 90.83 kJ mol-1 and 18.81 kJ mol-1, respectively. Moreover, a novel CO2-derived HCO4--based system led to a comparable acetaminophen degradation efficiency of 82 % and a higher kobs of 0.028 min-1. The system optimization and ROS evaluation suggest that high concentration of H2O2 inhibited the degradation and quenched CO3· and ·OH to yield ·O2- and 1O2. Furthermore, EPR analysis and quenching experiments indicate that CO3· was mainly responsible for acetaminophen degradation. This work provides fundamental understanding of the HCO4--based oxidation system.
利用 HCO3- 和 H2O2 反应生成的过氧化单碳酸盐(HCO4-)的高级氧化工艺,被用于去除水中的污染物。然而,H2O2 在这些过程中的确切作用仍是一个争论的话题。本研究利用 NaHCO3 和 H2O2 建立了一个基于 HCO4 的氧化系统来降解对乙酰氨基酚,并研究了共存氧化剂的活化机制。在热激活条件下,HCO4-(HO-OCOO-)中的O-O键比共存氧化剂H2O2(HO-OH)中的O-O键更容易裂解,从而产生活性氧(ROS)。根据动力学和 ROS 评估,H2O2 主要用于形成 HCO4-,而不是转化为 -OH 或 O2,HCO4- 通过形成 CO3-- 和 -OH 成为降解的主要氧化剂。在该氧化体系中,20 mM HCO3- 和 20 mM H2O2 在 60 °C 条件下,产生 -OH 的 H2O2 利用率达到 27.34%,-OH 产量达到 24.15%,对乙酰氨基酚的降解效率达到 83%。计算得出的对乙酰氨基酚降解表观活化能和 HCO4- 活化表观活化能分别为 90.83 kJ mol-1 和 18.81 kJ mol-1。此外,基于 CO2 衍生 HCO4- 的新型系统的对乙酰氨基酚降解效率为 82%,Kobs 为 0.028 min-1。系统优化和 ROS 评估表明,高浓度 H2O2 可抑制降解,并淬灭 CO3-- 和 -OH 生成 -O2- 和 1O2。此外,EPR 分析和淬灭实验表明 CO3--是对乙酰氨基酚降解的主要原因。这项研究为了解基于 HCO4 的氧化系统提供了基础。
{"title":"Reconsideration of the role of hydrogen peroxide in peroxymonocarbonate-based oxidation system for pollutant control","authors":"Zihan Yang ,&nbsp;Yi Zhou ,&nbsp;Yiqian Jiang ,&nbsp;Peiqing Zhao ,&nbsp;Xu Meng","doi":"10.1016/j.watres.2024.122750","DOIUrl":"10.1016/j.watres.2024.122750","url":null,"abstract":"<div><div>Advanced oxidation processes that utilize peroxymonocarbonate (HCO<sub>4</sub><sup>-</sup>), generated in-situ through the reaction of HCO<sub>3</sub><sup>-</sup> and H<sub>2</sub>O<sub>2</sub>, are employed for the removal of pollutants in water. Nevertheless, the precise role of H<sub>2</sub>O<sub>2</sub> in these processes remains a subject of debate. This study established a HCO<sub>4</sub><sup>-</sup>-based oxidation system using NaHCO<sub>3</sub> and H<sub>2</sub>O<sub>2</sub> for the degradation of acetaminophen and investigated the activation mechanisms of coexisting oxidants. Under thermal activation conditions, the O<img>O bond in HCO<sub>4</sub><sup>-</sup> (HO<img>OCOO<sup>-</sup>) was more readily cleaved than the O<img>O bond in the co-existing oxidant H<sub>2</sub>O<sub>2</sub> (HO<img>OH), leading to the generation of reactive oxygen species (ROS). Based on kinetics and ROS evaluation, H<sub>2</sub>O<sub>2</sub> primarily served to form HCO<sub>4</sub><sup>-</sup> rather than converting to ·OH or O<sub>2</sub>, with HCO<sub>4</sub><sup>-</sup> acting as the primary oxidant for degradation through the formation of <span><math><msubsup><mtext>CO</mtext><mrow><mn>3</mn></mrow><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></math></span>and <strong>·</strong>OH. In this oxidation system, H<sub>2</sub>O<sub>2</sub> utilization efficiency for <strong>·</strong>OH production reached 27.34 %, <strong>·</strong>OH yield reached 24.15 % and acetaminophen degradation efficiency realized 83 % at 60 °C with 20 mM HCO<sub>3</sub><sup>-</sup> and 20 mM H<sub>2</sub>O<sub>2</sub>. The apparent activation energy of acetaminophen degradation and HCO<sub>4</sub><sup>-</sup> activation were calculated as 90.83 kJ mol<sup>-1</sup> and 18.81 kJ mol<sup>-1</sup>, respectively. Moreover, a novel CO<sub>2</sub>-derived HCO<sub>4</sub><sup>-</sup>-based system led to a comparable acetaminophen degradation efficiency of 82 % and a higher k<em><sub>obs</sub></em> of 0.028 min<sup>-1</sup>. The system optimization and ROS evaluation suggest that high concentration of H<sub>2</sub>O<sub>2</sub> inhibited the degradation and quenched <span><math><msubsup><mtext>CO</mtext><mrow><mn>3</mn></mrow><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></math></span> and <strong>·</strong>OH to yield <strong>·</strong>O<sub>2</sub><sup>-</sup> and <sup>1</sup>O<sub>2</sub>. Furthermore, EPR analysis and quenching experiments indicate that <span><math><msubsup><mtext>CO</mtext><mrow><mn>3</mn></mrow><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></math></span> was mainly responsible for acetaminophen degradation. This work provides fundamental understanding of the HCO<sub>4</sub><sup>-</sup>-based oxidation system.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122750"},"PeriodicalIF":11.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142579841","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}
引用次数: 0
Heating and ultraviolet irradiation: Gas pressure meter-based analytical system for on-site and rapid monitoring of permanganate index (CODMn) 加热和紫外线照射:现场快速监测高锰酸盐指数(CODMn)的基于气体压力计的分析系统
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-05 DOI: 10.1016/j.watres.2024.122758
Jiayuan Tang , Dali Zhuo , Jihong Chen , Jing Xiao , Ronghua Zeng , Chao Tan , Xiaoli Xiong , Zhirong Zou
Permanganate index (CODMn) is one of the important indicators of surface water quality measurement. Herein, a portable analytical system was developed for on-site and rapid analysis of CODMn, organic substances in water were oxidized and transformed into gases, so that CODMn concentration was converted into a change of gas pressure signal, the pressure signal change was further detected by a gas pressure meter. Heating method and ultraviolet (UV) irradiation method were used as assisting technologies for oxidization of organic substances by acidic KMnO4, a linear range of 2–150 mg l-1 and a detectable limit of 2 mg l-1 were obtained. Those methods were further applied to the detection of CODMn in various water samples (lake waters and domestic sewage) and certified reference water samples (BWZ 6974–2016C and BWZ 7617–2016), with recoveries of 89–111 %. Among them, a portable analytical system based on UV irradiation gas pressure meter was further established and used for the analysis of CODMn in field. It is a promising analytical system/device for CODMn monitoring in field, offering advantages of low-cost, easy-operation, portability and rapidness.
高锰酸盐指数(CODMn)是地表水水质测量的重要指标之一。本文开发了一种用于现场快速分析 CODMn 的便携式分析系统,将水中的有机物氧化并转化为气体,从而将 CODMn 浓度转化为气体压力信号的变化,压力信号的变化由气体压力计进一步检测。采用加热法和紫外线(UV)照射法作为酸性 KMnO4 氧化有机物的辅助技术,获得了 2-150 mg L-1 的线性范围和 2 mg L-1 的检测限。将这些方法进一步应用于各种水样(湖水和生活污水)和认证参考水样(BWZ 6974-2016C 和 BWZ 7617-2016)中 CODMn 的检测,回收率为 89-111%。其中,基于紫外照射气体压力计的便携式分析系统被进一步建立并用于现场分析 CODMn。该分析系统/设备具有成本低、操作简便、便携快速等优点,是一种很有前景的 CODMn 现场监测分析系统/设备。
{"title":"Heating and ultraviolet irradiation: Gas pressure meter-based analytical system for on-site and rapid monitoring of permanganate index (CODMn)","authors":"Jiayuan Tang ,&nbsp;Dali Zhuo ,&nbsp;Jihong Chen ,&nbsp;Jing Xiao ,&nbsp;Ronghua Zeng ,&nbsp;Chao Tan ,&nbsp;Xiaoli Xiong ,&nbsp;Zhirong Zou","doi":"10.1016/j.watres.2024.122758","DOIUrl":"10.1016/j.watres.2024.122758","url":null,"abstract":"<div><div>Permanganate index (COD<sub>Mn</sub>) is one of the important indicators of surface water quality measurement. Herein, a portable analytical system was developed for on-site and rapid analysis of COD<sub>Mn</sub>, organic substances in water were oxidized and transformed into gases, so that COD<sub>Mn</sub> concentration was converted into a change of gas pressure signal, the pressure signal change was further detected by a gas pressure meter. Heating method and ultraviolet (UV) irradiation method were used as assisting technologies for oxidization of organic substances by acidic KMnO<sub>4</sub>, a linear range of 2–150 mg <span>l</span><sup>-1</sup> and a detectable limit of 2 mg <span>l</span><sup>-1</sup> were obtained. Those methods were further applied to the detection of COD<sub>Mn</sub> in various water samples (lake waters and domestic sewage) and certified reference water samples (BWZ 6974–2016C and BWZ 7617–2016), with recoveries of 89–111 %. Among them, a portable analytical system based on UV irradiation gas pressure meter was further established and used for the analysis of COD<sub>Mn</sub> in field. It is a promising analytical system/device for COD<sub>Mn</sub> monitoring in field, offering advantages of low-cost, easy-operation, portability and rapidness.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122758"},"PeriodicalIF":11.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580344","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}
引用次数: 0
Key process of ethanol hydrogen donor promoting the conversion of organic matter in sludge to bio-oil 乙醇供氢体促进污泥中有机物转化为生物油的关键过程
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-05 DOI: 10.1016/j.watres.2024.122753
Quxiu Dai , Linglong Zeng , Qihong Cen , Wang Du , Ping Ning , Kai Li , Zhiying Guo , Ran Ao , Longgui Xie , Nanqi Ren , Liping Ma , Jie Yang , Guocai Tian , Xin Sun
To develop clean energy utilization of sewage sludge, this study investigated the conversion behavior of organics and energy in supercritical sludge-ethanol system. The influence of liquefied parameters on products distribution, hydrogen supply process of ethanol for sludge liquefaction, migration of organics, and energy transformation were investigated. Results indicated that ethanol acted as both a solvent and a hydrogen donor. It providing H⋅ to promote organics dissociation for bio-oil production through radical reactions. Formation of new products in bio-oil such as C20H38O2 and C20H38O2 may be caused by H⋅ generated from OH and CH in ethanol. The increase in dodecanes and hexadecanes in bio-oil may be formed by recombination of smaller radicals such as HO·, H·, CH3⋅, CH3CH2⋅ from dissociation of ethanol and organics. Additionally, energy migration process indicated that higher temperatures increased carbon content in bio-oil from 40.88 to 48.92 %, decreased oxygen content from 48.6 to 39.56 %, and raised the calorific value of bio-oil from 29.63 to 30.11 MJ/kg. Besides, approximately 74.14 % of sludge energy transferred to bio-oil, while about 71.94 % of oxygen moved to bio-char, reducing the calorific value of bio-char to 0.03 MJ/kg. Notably, about 240.5 kg of bio-oil can be produced from 1t of sludge, reducing net carbon emissions by 43.583 kg, and presenting a sustainable alternative to fossil fuels. This study innovatively investigated the dual role of ethanol for sludge liquefaction, providing an efficient and sustainable method for energy recovery from sludge.
为开发污水污泥的清洁能源利用,本研究探讨了超临界污泥-乙醇系统中有机物和能量的转化行为。研究了液化参数对产物分布的影响、乙醇对污泥液化的供氢过程、有机物的迁移以及能量转化。结果表明,乙醇既是溶剂,又是氢供体。它通过自由基反应提供氢⋅以促进生物油生产中的有机物解离。生物油中新产物(如 C20H38O2 和 C20H38O2)的形成可能是由乙醇中的-OH 和-CH 产生的氢⋅引起的。生物油中十二烷和十六烷的增加可能是乙醇和有机物解离产生的较小自由基(如 HO-、H-、CH3⋅、CH3CH2⋅)重组形成的。此外,能量迁移过程表明,温度越高,生物油中的碳含量从 40.88% 增加到 48.92%,氧含量从 48.6% 降低到 39.56%,生物油的热值从 29.63 兆焦/千克提高到 30.11 兆焦/千克。此外,约 74.14% 的污泥能量转移到生物油中,约 71.94% 的氧气转移到生物炭中,生物炭的热值降低到 0.03 兆焦/千克。值得注意的是,1 吨污泥可生产约 240.5 千克生物油,净碳排放量减少 43.583 千克,是化石燃料的可持续替代品。这项研究创新性地探讨了乙醇在污泥液化中的双重作用,为从污泥中回收能源提供了一种高效、可持续的方法。
{"title":"Key process of ethanol hydrogen donor promoting the conversion of organic matter in sludge to bio-oil","authors":"Quxiu Dai ,&nbsp;Linglong Zeng ,&nbsp;Qihong Cen ,&nbsp;Wang Du ,&nbsp;Ping Ning ,&nbsp;Kai Li ,&nbsp;Zhiying Guo ,&nbsp;Ran Ao ,&nbsp;Longgui Xie ,&nbsp;Nanqi Ren ,&nbsp;Liping Ma ,&nbsp;Jie Yang ,&nbsp;Guocai Tian ,&nbsp;Xin Sun","doi":"10.1016/j.watres.2024.122753","DOIUrl":"10.1016/j.watres.2024.122753","url":null,"abstract":"<div><div>To develop clean energy utilization of sewage sludge, this study investigated the conversion behavior of organics and energy in supercritical sludge-ethanol system. The influence of liquefied parameters on products distribution, hydrogen supply process of ethanol for sludge liquefaction, migration of organics, and energy transformation were investigated. Results indicated that ethanol acted as both a solvent and a hydrogen donor. It providing H⋅ to promote organics dissociation for bio-oil production through radical reactions. Formation of new products in bio-oil such as C<sub>20</sub>H<sub>38</sub>O<sub>2</sub> and C<sub>20</sub>H<sub>38</sub>O<sub>2</sub> may be caused by H⋅ generated from <img>OH and <img>CH in ethanol. The increase in dodecanes and hexadecanes in bio-oil may be formed by recombination of smaller radicals such as HO·, H·, CH<sub>3</sub>⋅, CH<sub>3</sub>CH<sub>2</sub>⋅ from dissociation of ethanol and organics. Additionally, energy migration process indicated that higher temperatures increased carbon content in bio-oil from 40.88 to 48.92 %, decreased oxygen content from 48.6 to 39.56 %, and raised the calorific value of bio-oil from 29.63 to 30.11 MJ/kg. Besides, approximately 74.14 % of sludge energy transferred to bio-oil, while about 71.94 % of oxygen moved to bio-char, reducing the calorific value of bio-char to 0.03 MJ/kg. Notably, about 240.5 kg of bio-oil can be produced from 1t of sludge, reducing net carbon emissions by 43.583 kg, and presenting a sustainable alternative to fossil fuels. This study innovatively investigated the dual role of ethanol for sludge liquefaction, providing an efficient and sustainable method for energy recovery from sludge.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122753"},"PeriodicalIF":11.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142579840","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}
引用次数: 0
Structure-activity relationship between crystal plane and pyrite-driven autotrophic denitrification efficacy: Electron transfer and metagenome-based microbial mechanism 晶体平面与黄铁矿驱动的自养反硝化功效之间的结构-活性关系:电子传递和基于元基因组的微生物机制
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-05 DOI: 10.1016/j.watres.2024.122756
Yingmu Wang , Shi Chen , Yuanjing Chen , Junge Xu , Jian Zhou , Qiang He , Ziyuan Lin , Kai-qin Xu , Gongduan Fan
Pyrite-driven autotrophic denitrification (PAD) has been recognized as a promising treatment technology for nitrate removal. Although the occurrence of PAD has been found in recent years, there is a knowledge gap about effects of crystal plane of pyrite on the performance and mechanism of PAD system. Here, this study investigated the effects of crystal planes ({100}, {111} and {210}) of single-crystal pyrite on denitrification performance, electron transfer, and microbial mechanism in PAD system. The removal efficiency of nitrate in B-{210} reached 100%, which was 1.67-fold and 2.86-fold higher than that of B-{100} and B-{111}, respectively. X-ray photoelectron spectroscopy and electrochemical results indicated that Fe-S bonds of pyrite with {210} crystal plane were more susceptible to breakage by Fe3+ oxidation assault, and leaching microbially available Fe2+ and sulfur intermediates to drive autotrophic denitrification. Metagenomic results suggested that community of functional pyrite-driven denitrifiers varied in response to crystal plane, and abundances of N-S transformation and EET-related microbes and genes in B-{210} notably up-regulated compared to B-{100} and B-{111}. In addition, this work proposed a dual-mode for electron transfer pathway during pyrite oxidation and nitrogen transformation in PAD system. In B-{210}, Fe(II)- and sulfur-driven denitrifiers obtained electron after pyrite oxidation-dissolution, and the enrichment of pyrite-oxidizing bacteria in B-{210} could enhance the electron transfer from pyrite through electron shuttles. This work highlighted that stronger surface reactivity and electron shuttle effect in B-{210} enhanced electron transfer, leading to favorable PAD performance in B-{210}. Overall, this study provides novel insights into the structure-activity relationship between the crystal plane structure of pyrite and denitrification activity in PAD system.
黄铁矿驱动的自养反硝化(PAD)被认为是一种很有前景的硝酸盐去除处理技术。虽然近年来发现了黄铁矿自养反硝化现象,但关于黄铁矿晶面对自养反硝化系统性能和机理的影响还存在知识空白。本研究探讨了单晶黄铁矿的晶面({100}、{111}和{210})对 PAD 系统中脱硝性能、电子传递和微生物机理的影响。B-{210}对硝酸盐的去除率达到100%,分别是B-{100}和B-{111}的1.67倍和2.86倍。X射线光电子能谱和电化学结果表明,{210}晶面的黄铁矿的Fe-S键更容易被Fe3+氧化作用破坏,并浸出微生物可利用的Fe2+和硫中间产物,从而驱动自养反硝化作用。元基因组学结果表明,黄铁矿驱动的功能性反硝化菌群落随晶面的变化而变化,与B-{100}和B-{111}相比,B-{210}中N-S转化和EET相关微生物和基因的丰度明显上调。此外,这项研究还提出了PAD系统中黄铁矿氧化和氮转化过程中电子传递途径的双重模式。在B-{210}中,铁(II)和硫驱动的反硝化菌在黄铁矿氧化溶解后获得电子,而B-{210}中黄铁矿氧化菌的富集可通过电子穿梭器加强黄铁矿的电子传递。这项工作突出表明,B-{210}中更强的表面活性和电子穿梭效应增强了电子传递,从而使B-{210}具有良好的PAD性能。总之,本研究为黄铁矿晶体平面结构与 PAD 系统中脱硝活性之间的结构-活性关系提供了新的见解。
{"title":"Structure-activity relationship between crystal plane and pyrite-driven autotrophic denitrification efficacy: Electron transfer and metagenome-based microbial mechanism","authors":"Yingmu Wang ,&nbsp;Shi Chen ,&nbsp;Yuanjing Chen ,&nbsp;Junge Xu ,&nbsp;Jian Zhou ,&nbsp;Qiang He ,&nbsp;Ziyuan Lin ,&nbsp;Kai-qin Xu ,&nbsp;Gongduan Fan","doi":"10.1016/j.watres.2024.122756","DOIUrl":"10.1016/j.watres.2024.122756","url":null,"abstract":"<div><div>Pyrite-driven autotrophic denitrification (PAD) has been recognized as a promising treatment technology for nitrate removal. Although the occurrence of PAD has been found in recent years, there is a knowledge gap about effects of crystal plane of pyrite on the performance and mechanism of PAD system. Here, this study investigated the effects of crystal planes ({100}, {111} and {210}) of single-crystal pyrite on denitrification performance, electron transfer, and microbial mechanism in PAD system. The removal efficiency of nitrate in <em>B-{210}</em> reached 100%, which was 1.67-fold and 2.86-fold higher than that of <em>B-{100}</em> and <em>B-{111}</em>, respectively. X-ray photoelectron spectroscopy and electrochemical results indicated that Fe-S bonds of pyrite with {210} crystal plane were more susceptible to breakage by Fe<sup>3+</sup> oxidation assault, and leaching microbially available Fe<sup>2+</sup> and sulfur intermediates to drive autotrophic denitrification. Metagenomic results suggested that community of functional pyrite-driven denitrifiers varied in response to crystal plane, and abundances of N-S transformation and EET-related microbes and genes in <em>B-{210}</em> notably up-regulated compared to <em>B-{100}</em> and <em>B-{111}</em>. In addition, this work proposed a dual-mode for electron transfer pathway during pyrite oxidation and nitrogen transformation in PAD system. In <em>B-{210}</em>, Fe(II)- and sulfur-driven denitrifiers obtained electron after pyrite oxidation-dissolution, and the enrichment of pyrite-oxidizing bacteria in <em>B-{210}</em> could enhance the electron transfer from pyrite through electron shuttles. This work highlighted that stronger surface reactivity and electron shuttle effect in <em>B-{210}</em> enhanced electron transfer, leading to favorable PAD performance in <em>B-{210}</em>. Overall, this study provides novel insights into the structure-activity relationship between the crystal plane structure of pyrite and denitrification activity in PAD system.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122756"},"PeriodicalIF":11.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580343","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}
引用次数: 0
Forecasting nitrous oxide emissions from a full-scale wastewater treatment plant using LSTM-based deep learning models 利用基于 LSTM 的深度学习模型预测全规模污水处理厂的氧化亚氮排放量
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-05 DOI: 10.1016/j.watres.2024.122754
Siddharth Seshan , Johann Poinapen , Marcel H. Zandvoort , Jules B. van Lier , Zoran Kapelan
Nitrous oxide (N2O) emissions from wastewater treatment plants (WWTPs) exhibit significant seasonal variability, making accurate predictions with conventional biokinetic models difficult due to complex and poorly understood biochemical processes. This study addresses these challenges by exploring data-driven alternatives, using long short-term memory (LSTM) based encoder-decoder models as basis. The models were developed for future integration into a model predictive control framework, aiming to reduce N2O emissions by forecasting these over varying prediction horizons. The models were trained on 12 months and tested on 3 months of data from a full-scale WWTP in Amsterdam West, the Netherlands. The dataset encompasses seasonal peaks in N2O emissions typical for winter and spring months. The best performing model, featuring a 256–256 LSTM architecture, achieved the highest accuracy with test R2 values up to 0.98 across prediction horizons spanning 0.5 to 6.0 h ahead. Feature importance analysis identified past N2O emissions, influent flowrate, NH4+, NOx, and dissolved oxygen (DO) in the aerobic tank as most significant inputs. The observed decreasing influence of historical N2O emissions over extended prediction horizons highlights the importance and significance of process variables for the model's performance. The model's ability to accurately forecast short-term N2O emissions and capture immediate trends highlights its potential for operational use in controlling emissions in WWTPs. Further research incorporating diverse datasets and biochemical process inputs related to microbial activities in the N2O production pathways could improve the model's accuracy for longer forecasting horizons. These findings advocate for hybridising deep learning models with biokinetic and mechanistic insights to enhance prediction accuracy and interpretability.
污水处理厂(WWTPs)的氧化亚氮(N2O)排放具有显著的季节性变化,由于生化过程复杂且鲜为人知,因此传统的生物动力学模型很难进行准确预测。本研究以基于长短期记忆(LSTM)的编码器-解码器模型为基础,通过探索数据驱动的替代方法来应对这些挑战。开发这些模型是为了将来集成到模型预测控制框架中,目的是通过预测不同预测范围内的 N2O 排放量来减少排放。模型在荷兰阿姆斯特丹西区一个大型污水处理厂 12 个月的数据基础上进行了训练,并在 3 个月的数据基础上进行了测试。数据集包含了冬季和春季典型的 N2O 排放季节性峰值。性能最好的模型采用 256-256 LSTM 架构,在提前 0.5 到 6.0 小时的预测范围内,测试 R2 值高达 0.98,达到了最高准确度。特征重要性分析表明,过去的一氧化二氮排放量、进水流量、NH4+、氮氧化物和好氧池中的溶解氧 (DO) 是最重要的输入。观察到历史 N2O 排放量的影响随着预测时间的延长而减小,这凸显了工艺变量对模型性能的重要性和意义。该模型能够准确预测短期 N2O 排放量并捕捉即时趋势,这凸显了其在控制污水处理厂排放方面的应用潜力。进一步研究纳入与 N2O 生产途径中微生物活动相关的各种数据集和生化过程输入,可以提高该模型在更长预测期限内的准确性。这些研究结果主张将深度学习模型与生物动力学和机理见解相结合,以提高预测的准确性和可解释性。
{"title":"Forecasting nitrous oxide emissions from a full-scale wastewater treatment plant using LSTM-based deep learning models","authors":"Siddharth Seshan ,&nbsp;Johann Poinapen ,&nbsp;Marcel H. Zandvoort ,&nbsp;Jules B. van Lier ,&nbsp;Zoran Kapelan","doi":"10.1016/j.watres.2024.122754","DOIUrl":"10.1016/j.watres.2024.122754","url":null,"abstract":"<div><div>Nitrous oxide (N<sub>2</sub>O) emissions from wastewater treatment plants (WWTPs) exhibit significant seasonal variability, making accurate predictions with conventional biokinetic models difficult due to complex and poorly understood biochemical processes. This study addresses these challenges by exploring data-driven alternatives, using long short-term memory (LSTM) based encoder-decoder models as basis. The models were developed for future integration into a model predictive control framework, aiming to reduce N<sub>2</sub>O emissions by forecasting these over varying prediction horizons. The models were trained on 12 months and tested on 3 months of data from a full-scale WWTP in Amsterdam West, the Netherlands. The dataset encompasses seasonal peaks in N<sub>2</sub>O emissions typical for winter and spring months. The best performing model, featuring a 256–256 LSTM architecture, achieved the highest accuracy with test R<sup>2</sup> values up to 0.98 across prediction horizons spanning 0.5 to 6.0 h ahead. Feature importance analysis identified past N<sub>2</sub>O emissions, influent flowrate, NH<sub>4</sub><sup>+</sup>, NO<sub>x</sub>, and dissolved oxygen (DO) in the aerobic tank as most significant inputs. The observed decreasing influence of historical N<sub>2</sub>O emissions over extended prediction horizons highlights the importance and significance of process variables for the model's performance. The model's ability to accurately forecast short-term N<sub>2</sub>O emissions and capture immediate trends highlights its potential for operational use in controlling emissions in WWTPs. Further research incorporating diverse datasets and biochemical process inputs related to microbial activities in the N<sub>2</sub>O production pathways could improve the model's accuracy for longer forecasting horizons. These findings advocate for hybridising deep learning models with biokinetic and mechanistic insights to enhance prediction accuracy and interpretability.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122754"},"PeriodicalIF":11.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142579881","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
Water Research
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1