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Dual-functional FeMgAl-LDH/peroxydisulfate system for simultaneous carbon and phosphorus recovery from sludge anaerobic fermentation 双功能FeMgAl-LDH/过氧二硫酸钠系统在污泥厌氧发酵中同时回收碳和磷
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-01-01 DOI: 10.1016/j.watres.2026.125321
Dan Li , Yuxin Li , Wei Xia , Weixin Zhao , Xinhui Xia , Zixuan Zhao , Likui Feng , Heng Liang , Haijiao Xie , Liangliang Wei
The recovery of short-chain fatty acids (SCFAs) and phosphorus (P) from waste activated sludge (WAS) anaerobic fermentation is a promising sustainable strategy for resource valorization. However, its practical application has been hindered by low SCFAs yield and complex P recovery processes. In this study, a FeMgAl-layered double hydroxide (LDH)/peroxydisulfate (PDS) co-treatment strategy was proposed to overcome these challenges. FeMgAl-LDH effectively activated PDS to generate hydroxyl radicals (•OH) and sulfate radicals (SO4•−), leading to the disruption of extracellular polymeric substance and a 369.31% increase in dissolved organic matter (measured by SCOD), thus providing abundant substrates for SCFAs production. Furthermore, the system enhanced hydrolytic/acidogenic enzyme activity, enriched functional microbial communities, and activated acidogenic metabolic pathways. Consequently, SCFAs production increased by 7.90-fold (4598.56 vs. 582.27 mg COD/L), and the acetate proportion rose from 23.74% to 66.03%. Simultaneously, the co-treatment facilitated the release of both organic P and Fe-bound P, achieving a total P recovery efficiency of 21.28% via FeMgAl-LDH induced ion exchange, surface complexation, electrostatic attraction, and hydrogen bond. When used as a slow-release fertilizer, the recovered P-loaded FeMgAl-LDH increased the fresh weight of ryegrass by 51.02% in pot experiments. Overall, this synergistic strategy provides an innovative and integrated solution for simultaneous carbon and P resource recovery from WAS, highlighting its potential for advancing sustainable sludge management and circular bioeconomy practices.
从废活性污泥(WAS)厌氧发酵中回收短链脂肪酸(SCFAs)和磷(P)是一种有前途的可持续资源增值策略。然而,scfa产量低和P回收过程复杂阻碍了其实际应用。本研究提出了一种femgal层状双氢氧化物(LDH)/过硫酸氢盐(PDS)共处理策略来克服这些挑战。FeMgAl-LDH有效激活PDS生成羟基自由基(•OH)和硫酸盐自由基(SO4•−),导致细胞外聚合物质被破坏,溶解有机物(以SCOD测量)增加369.31%,从而为SCFAs的产生提供了丰富的底物。此外,该系统增强了水解/产酸酶活性,丰富了功能性微生物群落,激活了产酸代谢途径。结果表明,scfa产量提高了7.90倍(4598.56 mg /L vs 582.27 mg /L),乙酸比例从23.74%提高到66.03%。同时,通过FeMgAl-LDH诱导的离子交换、表面络合、静电吸引和氢键作用,共处理促进了有机磷和铁结合磷的释放,总磷回收率为21.28%。在盆栽试验中,作为缓释肥料,回收的富磷FeMgAl-LDH使黑麦草鲜重增加了51.02%。总体而言,这一协同战略为WAS同时回收碳和磷资源提供了一种创新的综合解决方案,突出了其在推进可持续污泥管理和循环生物经济实践方面的潜力。
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引用次数: 0
Hydrodynamics regulates microbial degradation of microplastics by modulating bottom-up and top-down effects in a river-lake confluence zone 水动力学通过调节河湖汇流区自下而上和自上而下的效应来调节微塑料的微生物降解
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-12-31 DOI: 10.1016/j.watres.2025.125311
Yamei Chen , Yi Li , Lihua Niu , Hans-Peter Grossart , Yingjie Wang , Xin Ma , Li Lin
River-lake confluence zones, characterized by unique hydrodynamic conditions, are critical areas for pollutant transformation. Nevertheless, degradation of microplastics (MP) mediated by multi-trophic microbial communities remains poorly understood under such complex hydrodynamic disturbances. This study investigated the characteristics of multi-trophic microbiota of the microplastome and explored their roles in MP degradation across four distinct hydrodynamic zones, i.e., maximum velocity zone (Z1), flow buffer zone (Z2), flow deflection zone (Z3), and flow reestablishment zone (Z4), in a river-lake confluence. A pronounced spatial heterogeneity in MP abundance and available nutrients was revealed among the four flow zones, with Z3 exhibiting the most intense MP degradation. Additional microcosm experiments demonstrated that microbial MP degradation was primarily driven by the enriched degrading bacteria and fungi, facilitated by multi-trophic microbial interactions. Furthermore, in situ analysis revealed that both bottom-up and top-down effects occurred across all flow zones, with their intensity being positively correlated with the degree of MP degradation. Thereby, nutrient availability driven by hydrodynamics stimulated the growth of MP degrading bacteria and fungi through a bottom-up effect. The increase in the relative abundance of MP degrading bacteria, concurrent with enhanced protozoan predation on bacteria, suggested that this top-down control operated through the selective predation of protozoa on non-MP degrading bacteria. Across the entire river-lake confluence zone, directional flow fluctuations were identified as the paramount environmental factor through the causal effect model, explaining >50% of the variance in bottom-up and top-down effects. Our study demonstrates how hydrodynamics governs MP degradation via multi-trophic microbial interactions, advancing our fundamental understanding of MP fate in aquatic ecosystems.
河湖汇流区具有独特的水动力条件,是污染物转化的关键区域。然而,在如此复杂的水动力扰动下,多营养微生物群落介导的微塑料(MP)降解仍然知之甚少。本研究研究了微质体的多营养菌群特征,并探讨了它们在最大流速区(Z1)、水流缓冲区(Z2)、水流偏折区(Z3)和水流重建区(Z4)四个不同水动力区中MP降解中的作用。4个流区MP丰度和速效养分存在明显的空间异质性,其中Z3区MP降解最为严重。其他微观实验表明,微生物降解MP主要由富集的降解细菌和真菌驱动,并由多营养微生物相互作用促进。此外,原位分析表明,自下而上和自上而下的影响都发生在所有流动区,其强度与MP降解程度呈正相关。因此,流体动力学驱动的养分有效性通过自下而上的效应刺激了MP降解细菌和真菌的生长。MP降解细菌相对丰度的增加,同时原生动物对细菌的捕食增强,表明这种自上而下的控制是通过原生动物对非MP降解细菌的选择性捕食来实现的。在整个河湖汇流带,通过因果关系模型,确定了方向流量波动是最重要的环境因素,解释了自下而上和自上而下影响差异的50%。我们的研究展示了水动力学如何通过多营养微生物的相互作用来控制MP的降解,促进了我们对水生生态系统中MP命运的基本理解。
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引用次数: 0
The driver of oil fate in nearshore environments: MOPAs-mediated vertical transport and ecotoxicity 近岸环境中石油命运的驱动因素:mopas介导的垂直运输和生态毒性
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-12-31 DOI: 10.1016/j.watres.2025.125264
Yuxiang Sun , Dongliang Lu , Xinping Wang , Ranran Dong , Jianing Yin , Guancheng Xie , Jinren Lu , Mutai Bao , Haoshuai Li
The vertical transport, including floating, sinking, suspending, and resuspending processes, and ecotoxicity of MPs-oil composite pollutants over long time scales significantly influence the fate of individual pollutants in nearshore environment. However, there is limited understanding of how multiple environmental factors influence vertical transport of MPs-oil composite pollutants. This study quantifies the effects of MPs properties on vertical-dimension distribution (focused on water columns and sediment phase) of different-viscosity oil and reveals related ecotoxicological impacts. A tenfold increase in MPs concentrations causes a 6.12% increase in average oil mass percentage (OMP) in sediment phase. Strong hydrophobicity of polyethylene maintains 52.60% oil in water columns, whereas weak adsorption of polyvinyl chloride promotes 69.44% oil distributed in sediment phase. High MPs concentrations facilitate oil distribution in sediment phase, resulting in lower OMP in water columns (29.65%) compared to sediment phase (70.35%). Regardless of MPs pollution levels, the concentration of oil mixtures in sediment phase is obviously higher than in water columns. The introduction of MPs into nearshore environments alters vertical transport and ecotoxicity of oil compared to MPs-free nearshore environment. Polyethylene increases mass of medium-long chain n-alkanes and polycyclic aromatic hydrocarbons in water columns by 737.68% and 41.99%, respectively. Conversely, particles adhering to the surface of MPs synergize with polyvinyl chloride to enhance its oil absorption capacity, thereby accelerating the accumulation of toxins and the mortality of benthic organisms in sediment phase. The aging of polyvinyl chloride enhances its adsorption capacity and promotes oil suspension, which impairs marine organism growth and development. These findings underscore the role of MOPAs in vertical transport and toxicity pathways of oil pollutants, providing a foundation for managing composite pollutants and maintaining marine ecosystem health.
在长时间尺度上,MPs-oil复合污染物的垂直迁移(包括漂浮、下沉、悬浮和再悬浮过程)和生态毒性显著影响着单个污染物在近岸环境中的命运。然而,对于多种环境因素如何影响MPs-oil复合污染物的垂直运移,人们的理解有限。本研究量化了MPs特性对不同黏度油垂直分布(以水柱和沉积物相为重点)的影响,揭示了相关的生态毒理学影响。MPs浓度增加10倍,导致沉积相平均油质量百分比(OMP)增加6.12%。聚乙烯的强疏水性维持了52.60%的油在水柱中的分布,而聚氯乙烯的弱吸附使69.44%的油在沉积物相中分布。高MPs浓度有利于油在沉积相中的分布,导致水柱的OMP(29.65%)低于沉积相(70.35%)。无论MPs污染程度如何,沉积物相的油混合物浓度明显高于水柱。与不含MPs的近岸环境相比,将MPs引入近岸环境会改变石油的垂直运输和生态毒性。聚乙烯使水柱中长链正构烷烃和多环芳烃的质量分别提高了737.68%和41.99%。相反,附着在MPs表面的颗粒与聚氯乙烯协同作用,增强其吸油能力,从而加速毒素的积累,加速底栖生物在沉积阶段的死亡。聚氯乙烯的老化使其吸附能力增强,产生浮油,不利于海洋生物的生长发育。这些发现强调了MOPAs在石油污染物垂直运移和毒性途径中的作用,为管理复合污染物和维持海洋生态系统健康提供了基础。
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引用次数: 0
Unveiling the adsorptive/catalytic roles of micro-carbon sphere materials in antibiotic removal: Current status and perspectives 微碳球材料在抗生素去除中的吸附/催化作用:现状与展望
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-12-31 DOI: 10.1016/j.watres.2025.125293
Ning Wang , Wang-mi Chen , Qi Zhou , Yu Dong , Ming-xiao Li , Bei-dou Xi , Jia-qi Hou , Zhen-tao Cui
Antibiotics, as typical emerging contaminants with low concentrations, require advanced adsorption/degradation technologies to mitigate their ecological and health risks. With remarkable adsorptive and catalytic properties, micro-carbon sphere (MCS) materials have emerged as potential candidates for promoting the antibiotic adsorption/degradation. Hence, a comprehensive understanding of the roles of MCS in antibiotic adsorption/degradation is crucial for developing applicable antibiotic removal technologies. This critical review systematically evaluates the triple advantage of MCS including hierarchical structure, surface properties, and tailored functionality, reveals their synthesis process, modification methods, as in enhancing different adsorption/degradation technologies, and identifies primary adsorption mechanisms including π–π interactions, electrostatic interactions, hydrogen bonding, and pore filling, and catalytic mechanism via promoting the generation of highly reactive free radicals. This study also reveals that the synergistic degradation mechanism occurs when MCS are combined with advanced oxidation processes and biological treatment technologies. However, limited material stability during MCS application, interference from organic interferents, inorganic ions, and physical clogging. Future research should prioritize exploring green and scalable preparation techniques, as well as advancing precise functional design tailored to specific antibiotics. By bridging material science with pollutant removal, this review presents actionable antibiotic removal technologies by using MCS as well as advancing the MCS toward practical application.
抗生素作为典型的低浓度新兴污染物,需要先进的吸附/降解技术来减轻其生态和健康风险。微碳球(MCS)材料具有显著的吸附和催化性能,是促进抗生素吸附/降解的潜在候选材料。因此,全面了解MCS在抗生素吸附/降解中的作用对于开发适用的抗生素去除技术至关重要。这篇综述系统地评价了MCS的三重优势,包括层次结构、表面性质和个性化功能,揭示了MCS的合成过程、改性方法,以增强不同的吸附/降解技术,并确定了主要的吸附机制,包括π -π相互作用、静电相互作用、氢键和孔隙填充,以及通过促进高活性自由基的产生的催化机制。该研究还揭示了MCS与高级氧化工艺和生物处理技术相结合时的协同降解机制。然而,在MCS应用过程中,材料的稳定性有限,有机干扰,无机离子和物理堵塞的干扰。未来的研究应优先探索绿色和可扩展的制备技术,并推进针对特定抗生素的精确功能设计。通过材料科学与污染物去除的结合,本文综述了可操作的MCS抗生素去除技术,并推动了MCS的实际应用。
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引用次数: 0
Sources of methylmercury in freshwater suspended particulate matter: Importance of In-situ methylation and adsorption 淡水悬浮颗粒物中甲基汞的来源:原位甲基化和吸附的重要性
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-12-31 DOI: 10.1016/j.watres.2025.125310
Cong Yao , Zhiyi Dai , Jinping Xue , Yuping Xiang , Yongguang Yin , Shanyi Tian , Tao Jiang , Yongmin Wang , Yong Cai , Dingyong Wang
Suspended particulate matter (SPM) plays a pivotal role in the transport and biogeochemical cycling of methylmercury (MeHg) in freshwater ecosystems. However, the trophic bioavailability and dominant sources of SPM-associated MeHg remain poorly characterized, limiting our understanding of its ecological impacts. This study conducted a comparative analysis of five representative freshwater systems in Southwest China, comprising three lakes and two rivers, to elucidate system-specific dynamics of SPM-associated MeHg. Results indicate that SPM contained substantially higher total MeHg concentrations and trophic-bioavailable fractions than surficial sediments. Remarkably, lake SPM accounted for 48.9% of the trophic-available MeHg in surficial sediment inventories, significantly higher than the contribution of river SPM (10.9%), underscoring the central role of lake systems as reservoirs of trophic-available MeHg and amplifiers of food web exposure. In lakes, MeHg in organic-rich SPM originated predominantly from in-situ methylation and aqueous-phase adsorption, with minimal contributions from sediment resuspension. Conversely, river SPM accumulated MeHg primarily through adsorption processes, reflecting distinct source mechanisms between the two systems. These findings challenge conventional paradigms that prioritize sediment resuspension as the dominant MeHg source in freshwater SPM and highlight the critical role of water-column processes, particularly in lacustrine environments, in driving SPM-associated MeHg dynamics. Altogether, these insights have profound implications for assessing trophic transfer risks and managing Hg contamination in aquatic environments.
悬浮颗粒物(SPM)在淡水生态系统中甲基汞(MeHg)的转运和生物地球化学循环中起着关键作用。然而,spm相关甲基汞的营养生物利用度和主要来源的特征仍然很差,限制了我们对其生态影响的理解。本研究通过对西南地区5个代表性淡水系统(3湖2河)的对比分析,阐明了与spm相关的MeHg的系统特异性动态。结果表明,表层沉积物中MeHg的总浓度和营养生物有效组分明显高于表层沉积物。值得注意的是,湖泊SPM占表层沉积物中营养有效MeHg的48.9%,显著高于河流SPM的贡献(10.9%),突出了湖泊系统作为营养有效MeHg储存库和食物网暴露放大器的核心作用。在湖泊中,富有机质SPM中的MeHg主要来源于原位甲基化和水相吸附,沉积物再悬浮的贡献很小。相反,河流SPM主要通过吸附过程积累MeHg,反映了两个系统之间不同的来源机制。这些发现挑战了将沉积物再悬浮作为淡水SPM中主要MeHg来源的传统范式,并强调了水柱过程(特别是湖泊环境)在驱动SPM相关MeHg动力学中的关键作用。总之,这些见解对评估营养转移风险和管理水生环境中的汞污染具有深远的意义。
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引用次数: 0
Regulation of photogenerated electron transfer efficiency: Heterojunction enhanced photocatalysis coupled with anaerobic ammonium oxidation for nitrogen removal 光生电子转移效率的调节:异质结增强光催化与厌氧氨氧化耦联去除氮
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-12-31 DOI: 10.1016/j.watres.2025.125309
Jing Yang , Chunhua He , Zhen-Hu Hu , Wei Wang
Anaerobic ammonium oxidation technologies are limited by nitrate accumulation in the treatment of wastewater with low carbon-to-nitrogen (C/N) ratios, making it difficult to achieve efficient total nitrogen removal. Light-driven biohybrid systems are promising emerging nitrate reduction technologies, yet the performance is limited by electron transfer efficiency. In this study, type II, Z-scheme, and S-scheme heterojunction photocatalysts, g-C3N4@CdS, were synthesized and coupled with anaerobic ammonium oxidation bacteria (AnAOB) to construct a light-driven biohybrid system capable of simultaneously removing nitrate and ammonium through enhanced photogenerated electron transfer. Among them, the S-scheme heterojunction photocatalyst with unique internal electric field and band bending configuration, exhibited the most effective charge separation and redox capability, achieving a total nitrogen removal efficiency of 94.8% under intermittent light without organic carbon. The electron transfer system activity increased by 335.2% and charge transfer resistance decreased by 7.4-fold, confirming the improved electron transfer efficiency in the S-scheme heterojunction system. The binding of light stimulation to the S-scheme heterojunction significantly increased the abundance of functional genes associated with the electron transport chain (e.g., CYTB, cydB, and ccoQ), thereby enhancing ATP synthesis and energy metabolism. The same phenomenon was observed in the abundance of denitrification-related genes (nar and nirS) and anaerobic ammonium oxidation genes (hzsA and hdh). This study elucidates the critical role of heterojunction structural regulation in facilitating electron transfer at the semiconductor-microbe interface and provides new insights and technical support for achieving efficient light-driven nitrogen removal from low C/N-ratio wastewater.
厌氧氨氧化技术在处理低碳氮比(C/N)废水时受到硝酸盐积累的限制,难以实现高效的总氮去除。光驱动生物混合系统是新兴的硝酸盐还原技术,但其性能受到电子转移效率的限制。在本研究中,合成了II型、z型和s型异质结光催化剂g-C3N4@CdS,并与厌氧氨氧化细菌(AnAOB)偶联,构建了一个通过增强光生电子转移同时去除硝酸盐和铵的光驱动生物杂化体系。其中,s型异质结光催化剂具有独特的内部电场和能带弯曲结构,在无有机碳的间歇光下,具有最有效的电荷分离和氧化还原能力,总氮去除效率为94.8%。电子转移体系活度提高了335.2%,电荷转移电阻降低了7.4倍,证实了s型异质结体系中电子转移效率的提高。光刺激与s型异质结的结合显著增加了与电子传递链相关的功能基因(如CYTB、cydB和ccoQ)的丰度,从而增强了ATP的合成和能量代谢。在反硝化相关基因(nar和nirS)和厌氧氨氧化基因(hzsA和hdh)的丰度中也观察到同样的现象。本研究阐明了异质结结构调控在促进半导体-微生物界面电子转移中的关键作用,为实现低碳氮比废水的高效光驱脱氮提供了新的见解和技术支持。
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引用次数: 0
Freezing prevents ⁶⁰Co‑γ irradiation artefacts in DOM concentration, composition and δ¹³C 冻结可防止6⁰Co‑γ辐照人工制品中的DOM浓度、成分和δ¹³C
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-12-31 DOI: 10.1016/j.watres.2025.125308
Elizabeth F. Bell , Karina T. Meredith , Justin B. Davies , Liza K. McDonough
Gamma (γ)-irradiation is often used to sterilise environmental water samples for international transport and biosecurity compliance. However, its impact on the molecular and isotopic integrity of dissolved organic matter (DOM) remains poorly understood. Here, we assess the effects of γ-irradiation (50 kGy), a commonly used sterilisation technique for water samples arriving into Australia, on dissolved organic carbon (DOC) concentration, DOM composition, and stable isotopic signatures (δ¹³C, δ¹⁵N, δ¹⁸O, δ2H) in natural waters and Milli-Q water mixed with organic matter standards, comparing frozen-irradiated and unfrozen-irradiated samples. Irradiation, when applied to unfrozen water, led to significant (p < 0.05) DOC loss, oxidative fragmentation of humic-like fluorophores, and significant (p < 0.05) δ¹³C enrichment of residual DOC, consistent with preferential ¹²C oxidation. Low-molecular-weight acids and microbial protein-like components increased, while aromaticity declined. In contrast, frozen samples exhibited no significant changes in DOC, DOM composition, and δ¹³C, indicating that immobilisation of DOM in ice suppresses its oxidation. Gamma irradiation also caused acidification (ΔpH ≈ –0.5 to –0.8 units) and altered concentrations of SO₄ and NO₃, with a significant increase in SO₄ likely resulting from the oxidation of dissolved organic sulfur. These results demonstrate that freezing samples prior to γ-irradiation effectively preserves both molecular and isotopic integrity of DOM and DOC concentration and therefore should be considered as an effective technique to maintain the integrity of environmental water samples during sterilisation in biogeochemical studies.
伽马(γ)辐照通常用于对国际运输和生物安全合规的环境水样进行消毒。然而,它对溶解有机物(DOM)分子和同位素完整性的影响仍然知之甚少。在这里,我们评估了γ辐照(50 kGy)对天然水和ml - q水中溶解有机碳(DOC)浓度、DOM组成和稳定同位素特征(δ¹³C、δ¹5 N、δ¹⁸O、δ 2h)的影响,并比较了冷冻辐照和未冷冻辐照的样品。γ辐照是一种常用的水样灭菌技术,用于入境澳大利亚的水样。当辐照于未冻结的水时,导致显著的(p < 0.05) DOC损失,腐殖质样荧光团氧化碎裂,残留DOC显著的(p < 0.05) δ¹³C富集,符合优先的¹²C氧化。低分子量酸和微生物蛋白样成分增加,芳香性下降。相比之下,冷冻样品的DOC、DOM组成和δ¹³C没有显著变化,这表明DOM在冰中的固定抑制了它的氧化。伽马辐射也引起了酸化(ΔpH≈-0.5到-0.8个单位),并改变了SO₄和NO₃的浓度,其中SO₄的显著增加可能是由于溶解的有机硫的氧化。这些结果表明,在γ辐照前冷冻样品可以有效地保持DOM和DOC浓度的分子和同位素完整性,因此在生物地球化学研究中,应将其视为在灭菌过程中保持环境水样完整性的有效技术。
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引用次数: 0
New insights into the electron-transfer mechanism of Cr(VI) activation by carbon materials for simultaneously enhanced Cr(VI) detoxicate and acetaminophen oxidation: the role of defect structures 碳材料激活Cr(VI)同时增强Cr(VI)解毒和对乙酰氨基酚氧化的电子转移机制的新见解:缺陷结构的作用
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-12-30 DOI: 10.1016/j.watres.2025.125301
Ying Zhao , Bai Yang , Zhiyuan Liang , Hongbin Ji , Zifu Li
Hexavalent chromium (Cr(VI)) is a widely recognized toxic heavy metal pollutant, yet its intrinsic oxidative potential remains underutilized. The observation that Cr(V) generated during sulfite- or photocatalyst-mediated Cr(VI) reduction exhibits efficient oxidation of coexisting organic compounds has prompted exploration of potential Cr(VI)-based heterogeneous catalytic systems. Herein, waste polyethylene was upcycled via a controlled salt-template pyrolysis strategy to synthesize carbon nanoscale catalysts (LCSs) with engineered defect structures. These LCSs synergistically amplified the oxidative capacity of potassium dichromate (PCr), achieving rapid degradation of diverse organic micropollutants and concurrent Cr(VI)-to-Cr(III) reduction. Combined theoretical and experimental analyses demonstrate that vacancy defects function as intrinsic active sites, enhancing polarization charge distribution and electron density redistribution on LCSs surfaces to amplify interfacial reactivity and electron mobility. This defect-driven electronic modulation enables efficient charge transfer between acetaminophen (ACP) and PCr. Furthermore, life cycle and techno-economic analyses highlighted the enhanced environmental and economic merits of the LCSs/PCr system, exhibiting a two-thirds reduction in carbon emissions compared to conventional processes and a 50 % reduction in operational costs. This work reveals defect structures' critical role in Cr(VI) catalysis systems, redefining chromium pollution control through Cr(VI) repurposing as catalytic assets and advancing sustainable water decontamination.
六价铬(Cr(VI))是一种公认的有毒重金属污染物,但其固有的氧化潜能尚未得到充分利用。观察到亚硫酸盐或光催化剂介导的Cr(VI)还原过程中产生的Cr(V)对共存的有机化合物具有有效的氧化作用,这促使人们探索潜在的Cr(VI)基非均相催化体系。本研究通过盐模板热解策略对废聚乙烯进行升级利用,合成具有工程缺陷结构的碳纳米级催化剂(LCSs)。这些lcs协同放大了重铬酸钾(PCr)的氧化能力,实现了多种有机微污染物的快速降解和Cr(VI)到Cr(III)的同步还原。结合理论和实验分析表明,空位缺陷作为本征活性位点,增强了lcs表面的极化电荷分布和电子密度再分布,从而增强了界面反应性和电子迁移率。这种缺陷驱动的电子调制使对乙酰氨基酚(ACP)和PCr之间的有效电荷转移成为可能。此外,生命周期和技术经济分析强调了lcs /PCr系统的环境和经济优势,与传统工艺相比,碳排放量减少了三分之二,运营成本降低了50%。本研究揭示了缺陷结构在Cr(VI)催化系统中的关键作用,通过Cr(VI)作为催化资产的再利用,重新定义了铬污染控制,并推进了可持续的水净化。
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引用次数: 0
Up-scaling of a photoelectrochemical system with regulated chloride activation for negative-emission saline sewage treatment and disinfection byproduct mitigation 调节氯化物活化的光电化学系统用于负排放盐水污水处理和消毒副产物缓解的放大
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-12-30 DOI: 10.1016/j.watres.2025.125306
Zexiao Zheng , Justin H.K. Man , Howard Y.M. Cheung , Cheuk Wai Lung , Taoran Dong , Irene M.C. Lo
Conventional wastewater treatment plants (WWTPs) are carbon- and energy-intensive, inefficient in degrading emerging pollutants (EPs), and require additional chemicals. The photoelectrochemical (PEC) system offers a sustainable approach for saline sewage treatment; however, effective regulation of chloride activation and demonstration of scalability remain critical challenges. Herein, a bismuth- and oxygen-vacancies modified BiVO4 (BvOv-BVO) photoanode is developed to regulate chloride activation, efficiently removing chemical oxygen demand (including EP), ammonia-N, and bacteria from simulated saline sewage coupled with substantial H2 evolution, while suppressing 76.6% of disinfection byproduct (DBP) formation compared to BVO. Importantly, it achieves negative emissions through restrained greenhouse gas (GHG) generation and carbon offsets from green H2 evolution. Mechanistic investigations reveal that BvOv-BVO regulates chloride activation to generate ClO as the dominant reactive chlorine species, which simultaneously accelerates contaminant removal, suppresses DBP formation, and mitigates GHG emissions to enable negative emissions. To validate scalability, a continuous-flow prototypical PEC reactor with enlarged light absorption area, optimized light exposure, enhanced mass transfer, and improved hydrodynamics is established. This prototype exhibits exceptional performance in treating real saline sewage under natural sunlight, meeting discharge standards within 2 h, sustaining negative emissions and DBP control, and demonstrating excellent long-term stability. This study pioneers a scalable, negative-emission PEC system as a powerful and sustainable substitute for activated sludge and disinfection processes.
传统的污水处理厂(WWTPs)是碳和能源密集型的,在降解新污染物(EPs)方面效率低下,并且需要额外的化学品。光电化学(PEC)系统为含盐污水处理提供了一种可持续的方法;然而,氯化物活化的有效调控和可扩展性的证明仍然是关键的挑战。本研究开发了一种铋和氧空位修饰的BiVO4 (BvOv-BVO)光阳极,用于调节氯化物活化,有效去除模拟含盐污水中的化学需氧量(包括EP)、氨氮和细菌,同时与BVO相比,能抑制76.6%的消毒副产物(DBP)的形成。重要的是,它通过抑制温室气体(GHG)的产生和绿色氢气的碳抵消来实现负排放。机理研究表明,BvOv-BVO调节氯化物活化生成ClO•作为主要的活性氯,同时加速污染物去除,抑制DBP的形成,减轻温室气体排放,实现负排放。为了验证可扩展性,建立了一个扩大光吸收面积、优化光照射、增强传质和改善流体力学的连续流PEC反应器原型。该样机在自然光照下处理真实含盐污水,在2小时内达到排放标准,保持负排放和DBP控制,并表现出优异的长期稳定性。这项研究开创了一个可扩展的,负排放的PEC系统,作为活性污泥和消毒过程的强大和可持续的替代品。
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引用次数: 0
Microplastic-affected pathogens in drinking water supply systems: Survival mechanisms, ecological impacts and control challenges 饮用水供应系统中受微塑料影响的病原体:生存机制、生态影响和控制挑战
IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-12-30 DOI: 10.1016/j.watres.2025.125294
Ruidi Xu , Qiqi Wan , Ruihua Cao , Yanghui Xu , Huan Tang , Gang Liu , Gang Wen
Microplastics (MPs), as emerging pollutants, can affect pathogens, primarily opportunistic pathogens (OPs), and influence their behavior in aquatic environments. However, evidences regarding their impacts in drinking water supply systems (DWSSs) remain scarce. Focusing on the safety of DWSSs, this review synthesizes how MPs affect pathogen proliferation, transport, and resistance development under typical DWSS conditions characterized by low nutrients, high flow rates, oxidative stress, and user demand. MPs can distinctly promote the growth and reproduction of pathogens, act as mobile carriers enabling cross-watershed transport, and facilitate direct migration from source water to humans, thereby increasing health risks. Furthermore, MPs enhance pathogen resistance at both individual and community levels, thereby complicating subsequent control efforts. This study further summarizes how MPs compromise existing pathogen control measures in DWSSs and introduce secondary risks, including MP additives and the disinfection by-products from MPs. Finally, a strategy integrating “pretreatment interception” and “secondary risk reduction” is proposed to control MP-affected pathogens in DWSSs. The review provides valuable insights into mitigating pathogen risks associated with MPs in DWSSs, addressing a significant knowledge gap in safeguarding water security.
微塑料(MPs)作为新兴污染物,可以影响病原体,主要是机会致病菌(OPs),并影响其在水生环境中的行为。然而,它们对饮用水供应系统(dwss)的影响仍然很少。本文以DWSS的安全性为重点,综述了在低营养、高流速、氧化应激和用户需求的典型DWSS条件下,MPs是如何影响病原体增殖、运输和耐药性发展的。MPs可以明显促进病原体的生长和繁殖,作为移动载体实现跨流域运输,并促进从水源向人类的直接迁移,从而增加健康风险。此外,MPs增强了个体和社区层面的病原体耐药性,从而使后续控制工作复杂化。本研究进一步总结了MPs如何损害dwss中现有的病原体控制措施,并引入二次风险,包括MPs添加剂和MPs的消毒副产物。最后,提出了“预处理阻断”和“降低二次风险”相结合的策略来控制dwss中mp影响的病原体。该综述为减轻与dwss中MPs相关的病原体风险提供了有价值的见解,解决了维护水安全方面的重大知识缺口。
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