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Reconciling mass and number emissions through particle size: Implications for urban ultrafine particle modelling 通过颗粒大小协调质量和数量排放:对城市超细颗粒模型的影响
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-11-01 DOI: 10.1016/j.jhazmat.2026.143879
Soo-Jin Park,Lya Lugon,Youngseob Kim,Alexia Baudic,Amandine Rosso,Jeroen Kuenen,Marya el Malki,Karine Sartelet
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引用次数: 0
Abnormal electron-donation-dependent sulfite activation in the Mn(II)-nitrilotriacetic acid system: QSAR and mechanistic insights Mn(II)-硝基三乙酸体系中异常电子捐赠依赖的亚硫酸盐活化:QSAR和机制见解
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-10-29 DOI: 10.1016/j.jhazmat.2026.144070
Yanchanjuan Yang, Xinglian Qin, Pengli Zhang, Jiayu Wu, Shuaiqi Zhao, Xiuying Liu, Aihua Xu, Xiaoxia Li
In advanced oxidation processes (AOPs), electron-rich contaminants are generally susceptible to oxidation by reactive species. Herein, an unusual substrate-selective degradation was observed in sulfite (Na2SO3) based AOPs with the Mn(II)-nitrilotriacetic acid (NTA) complex. The strong electron-rich phenolics were hardly degraded, whereas electron-deficient phenols were efficiently removed. An asymmetric volcano-shaped correlation between the degradation rates and Hammett constants σ+ was established via quantitative structure-activity relationship analysis and can be expanded to antibiotics and dyes with anodic peak potential as a descriptor. Mechanistic investigations demonstrate that electron-rich phenolics complex with Mn(II)-NTA, suppressing O2-driven Mn(III)-NTA formation and thus limiting Mn(V)-NTA accumulation, with a slow radical chain reaction for Na2SO3 oxidation. In contrast, electron-deficient substrates promote Mn(III)-NTA generation, fast Na2SO3 oxidation and transformation to peroxymonosulfate (PMS), and subsequent Mn(V)-NTA formation. Consequently, radical pathways participate in the degradation of electron-rich pollutants, whereas Mn(V)-NTA governs the oxidation of electron-deficient ones. The low-cost Na2SO3 system shows comparable or superior performance to PMS-based systems for electron-deficient pollutants, highlighting its economic viability. These findings underscore the importance of pollutant-catalyst interactions in AOPs and provide mechanistic insights for targeted contaminant remediation.
在高级氧化过程(AOPs)中,富电子污染物通常容易被活性物质氧化。本文中,以亚硫酸盐(Na2SO3)为基础的AOPs与Mn(II)-nitrilotriacetic acid (NTA)配合物发生了不寻常的底物选择性降解。强富电子酚类化合物几乎不被降解,而缺电子酚类化合物则被有效地去除。通过定量构效关系分析,建立了降解速率与Hammett常数σ+之间的不对称火山型相关性,并将其推广到抗生素和染料中,以阳极峰电位作为描述符。机理研究表明,富电子酚类物质与Mn(II)-NTA络合,抑制o2驱动的Mn(III)-NTA的形成,从而限制Mn(V)-NTA的积累,并通过缓慢的自由基链反应氧化Na2SO3。相反,缺乏电子的底物促进Mn(III)-NTA生成,Na2SO3快速氧化并转化为过氧单硫酸盐(PMS),随后形成Mn(V)-NTA。因此,自由基途径参与富电子污染物的降解,而Mn(V)-NTA则控制缺电子污染物的氧化。低成本的Na2SO3系统表现出与基于pms的系统相当或更好的性能,突出了其经济可行性。这些发现强调了AOPs中污染物-催化剂相互作用的重要性,并为靶向污染物修复提供了机制见解。
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引用次数: 0
Molecular insight of U-As-Cd synergistic mineralization and metabolic responses mediated by Brevundimonas spp. 短单胞菌介导U-As-Cd协同矿化及代谢反应的分子机制。
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-10-29 DOI: 10.1016/j.jhazmat.2026.144075
Aishu Li, Lin Yu, Shuyan Mi, Zhongqiang Hu, Qi Liao, Weichun Yang, Qingzhu Li, Mengying Si, Nan Hu, Guangyue Li, Zhihui Yang
A novel promising environmentally friendly remediation method by As(III)-oxidizing bacteria has been demonstrated to facilitate the synergistic biomineralization for Uranium (U), Arsenic (As) and Cadmium (Cd). However, the underlying remediation mechanism remains unclear. Herein, the process of synergistic mineralization of U, As, and Cd and the metabolic response of Brevundimonas spp. were revealed. Brevundimonas spp. enhanced the synergistic removal efficiencies of 27.54, 18.17 and 19.93 times for U, As and Cd comparing with the chemical methods, respectively. Precipitates were formed initially on the bacterial cell surface, and gradually released into the extracellular matrix concomitant with a transformation from amorphous precursors to crystalline phases. The protein-protein interaction (PPI) results revealed that the proteins involved in the As(III) oxidation phase primarily mediated the interactions among electron transfer-related proteins. The addition of U and Cd further strengthened the link of electron transfer with the Na+/H+ transporter, ATPase, and superoxide dismutase (SOD). The expression differences in oxidative phosphorylation reflect the self-regulatory capacity of Brevundimonas spp. in response to heavy metal oxidation and synergistic mineralization. Our study provides a molecular insight by which As(III)-oxidizing bacteria enhance to simultaneously remove U, As and Cd in the mining wastewater.
利用As(III)氧化菌对铀(U)、砷(As)和镉(Cd)进行协同生物矿化处理是一种很有前景的环境友好型修复方法。然而,潜在的补救机制仍不清楚。本研究揭示了U、As和Cd协同矿化的过程以及Brevundimonas sp .的代谢反应。Brevundimonas对U、As和Cd的协同去除效率分别是化学方法的27.54倍、18.17倍和19.93倍。沉淀最初在细菌细胞表面形成,并逐渐释放到细胞外基质中,同时由无定形前体向结晶相转变。蛋白质-蛋白质相互作用(PPI)结果表明,参与As(III)氧化阶段的蛋白质主要介导电子转移相关蛋白之间的相互作用。U和Cd的加入进一步加强了电子转移与Na+/H+转运体、atp酶和超氧化物歧化酶(SOD)的联系。氧化磷酸化的表达差异反映了Brevundimonas sp .对重金属氧化和协同矿化的自我调节能力。我们的研究提供了As(III)氧化细菌增强同时去除采矿废水中U, As和Cd的分子视角。
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引用次数: 0
Biodegradable polylactic acid microplastics pose greater field nitrous oxide emission risks than conventional polyethylene by reshaping microbial production-reduction pathways in a wheat-maize rotation system 可生物降解聚乳酸微塑料通过重塑小麦-玉米轮作系统中微生物减产途径,比传统聚乙烯造成更大的田间氧化亚氮排放风险
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-10-29 DOI: 10.1016/j.jhazmat.2026.144068
Chuan Wang, Rui He, Lisha Wang, Yuan Li, Rui Li, Yiting Dai, Xiaoli He, Binghan Wang, Meng Yang, Xubo Wang
Microplastic contamination in agroecosystems is increasing, yet the field-scale effects of biodegradable microplastics on soil nitrous oxide (N2O) emissions remain unclear. We conducted a wheat–maize rotation field experiment to compare conventional polyethylene microplastics (PE-MPs) and biodegradable polylactic acid microplastics (PLA-MPs) at three application levels. Measurements included N2O fluxes, soil physicochemical properties, N-transformation enzyme activities, potential nitrification and denitrification rates, functional gene abundances, N2O/(N2O+N2) product ratios, 15N-18O-based N2O production pathways. Two-way ANOVA showed that microplastic type was the most consistent determinant of key responses, whereas concentration and interaction effects varied among indicators and seasons. PE-MPs caused weak and variable changes in soil N cycling and cumulative N2O emissions. In contrast, PLA-MPs increased cumulative N2O emissions by 38.9-61.1%, increased dissolved organic carbon, lowered pH, suppressed ammonia monooxygenase activity and nitrification, and stimulated nitrite reductase activity, potential denitrification, and nirK/nirS abundances. Increased N2O/(N2O+N2) and (nirK+nirS)/nosZ ratios indicated a stronger imbalance between N2O production and nosZ-mediated reduction. Dual-isotope tracing further showed that microplastics reduced nitrifier nitrification and shifted N2O production toward nitrifier denitrification, coupled nitrification–denitrification, and heterotrophic denitrification, with the strongest shift under PLA-MPs. These results demonstrate PLA-MPs pose greater N2O emission risks than PE-MPs, biodegradability does not necessarily imply environmental safety.
农业生态系统中的微塑料污染正在增加,但可生物降解微塑料对土壤一氧化二氮(N2O)排放的田间效应尚不清楚。通过小麦-玉米轮作试验,比较了常规聚乙烯微塑料(PE-MPs)和可生物降解聚乳酸微塑料(PLA-MPs)在三种施用水平下的差异。测量包括N2O通量、土壤物理化学性质、n转化酶活性、潜在的硝化和反硝化速率、功能基因丰度、N2O/(N2O+N2)产物比率、15n -18基N2O生产途径。双向方差分析显示,微塑性类型是关键响应的最一致的决定因素,而浓度和交互作用效应因指标和季节而异。PE-MPs对土壤N循环和累积N2O排放的影响是微弱和可变的。相比之下,PLA-MPs增加了累计N2O排放量38.9-61.1%,增加了溶解有机碳,降低了pH,抑制了氨单加氧酶活性和硝化作用,刺激了亚硝酸盐还原酶活性,潜在的反硝化作用和nirK/nirS丰度。N2O/(N2O+N2)和(nirK+nirS)/nosZ比值的增加表明N2O生成与nosZ介导的还原之间的不平衡加剧。双同位素示踪进一步表明,微塑料降低了硝化菌的硝化作用,并使N2O生产向硝化菌反硝化、硝化-反硝化耦合和异养反硝化方向转变,其中PLA-MPs的转变最为强烈。这些结果表明PLA-MPs比PE-MPs具有更大的N2O排放风险,生物可降解性并不一定意味着环境安全。
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引用次数: 0
Tailored nanofiltration membrane for enhanced performance by surface modification using zwitterionic piperazine 利用两性离子哌嗪对纳滤膜进行表面改性,提高纳滤膜的性能
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-10-29 DOI: 10.1016/j.jhazmat.2026.144045
Jincheng Ding, Chunyu Feng, Zongtang Liu, Zhihao Si, Qieyuan Gao
Nanofiltration (NF) membranes are indispensable for removing hazardous contaminants such as dyes and salts from industrial wastewater, yet their performance is often bottlenecked by the inherent permeability–selectivity trade-off and membrane fouling. Zwitterionic surface modification offers a means to overcome these limitations by promoting hydrophilicity and introducing charge-mediated transport. Here we synthesized a pre-formed zwitterionic piperazine (ZW-PIP) via a one-pot ring-opening of piperazine with 1,3-propanesultone, and directly grafted it onto polyamide films through residual acyl chloride groups. Combined low-field nuclear magnetic resonance (LF-NMR) and molecular dynamics (MD) simulations demonstrated that the grafted zwitterionic moieties stabilized a hydration layer and facilitated water and chloride-ion diffusion (>90%), while sterically excluding sulfate. The resulting membrane exhibited a pure water permeance of 29.2L∙m-2∙h-1∙bar-1. Crucially, this enhanced permeability was achieved while maintaining the exceptional salt-rejection performance for Na2SO4 (>97.0%). This high selectivity persisted even under challenging conditions of elevated salt concentration (8.0g/L) and operating pressure (8.0bar). The membrane exhibited robust rejection of various dyes (>96%), sustained stability, and potent antifouling (BSA, FRR 89%) and antibacterial (>99.97%) properties. Collectively, this work offers a mechanistic basis for designing zwitterionic NF membranes with high permeability, selectivity, and fouling resistance for treating complex hazardous wastewater.
纳滤膜是去除工业废水中染料、盐等有害污染物不可缺少的技术手段,但其性能往往受到固有的渗透性-选择性权衡和膜污染的制约。两性离子表面改性通过提高亲水性和引入电荷介导的输运,为克服这些限制提供了一种方法。本文通过哌嗪与1,3-丙磺酸的一锅开环,合成了预成型的两性离子哌嗪(ZW-PIP),并通过残留的酰基直接接枝到聚酰胺薄膜上。结合低场核磁共振(LF-NMR)和分子动力学(MD)模拟表明,接枝的两性离子部分稳定了水合层,促进了水和氯离子的扩散(>90%),同时在空间上排除了硫酸盐。所得膜的纯水渗透率为29.2L∙m-2∙h-1∙bar-1。至关重要的是,在提高渗透率的同时,还保持了Na2SO4优异的防盐性能(>97.0%)。即使在高盐浓度(8.0g/L)和操作压力(8.0bar)的挑战性条件下,这种高选择性仍然存在。该膜具有较强的对各种染料的去除率(>96%),持续的稳定性,以及有效的防污性能(BSA, FRR 89%)和抗菌性能(>99.97%)。本研究为设计具有高渗透性、选择性和抗污染性能的两性离子纳滤膜处理复杂有害废水提供了机理基础。
{"title":"Tailored nanofiltration membrane for enhanced performance by surface modification using zwitterionic piperazine","authors":"Jincheng Ding, Chunyu Feng, Zongtang Liu, Zhihao Si, Qieyuan Gao","doi":"10.1016/j.jhazmat.2026.144045","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2026.144045","url":null,"abstract":"Nanofiltration (NF) membranes are indispensable for removing hazardous contaminants such as dyes and salts from industrial wastewater, yet their performance is often bottlenecked by the inherent permeability–selectivity trade-off and membrane fouling. Zwitterionic surface modification offers a means to overcome these limitations by promoting hydrophilicity and introducing charge-mediated transport. Here we synthesized a pre-formed zwitterionic piperazine (ZW-PIP) via a one-pot ring-opening of piperazine with 1,3-propanesultone, and directly grafted it onto polyamide films through residual acyl chloride groups. Combined low-field nuclear magnetic resonance (LF-NMR) and molecular dynamics (MD) simulations demonstrated that the grafted zwitterionic moieties stabilized a hydration layer and facilitated water and chloride-ion diffusion (&gt;90%), while sterically excluding sulfate. The resulting membrane exhibited a pure water permeance of 29.2<ce:hsp sp=\"0.25\"></ce:hsp>L∙m<ce:sup loc=\"post\">-2</ce:sup>∙h<ce:sup loc=\"post\">-1</ce:sup>∙bar<ce:sup loc=\"post\">-1</ce:sup>. Crucially, this enhanced permeability was achieved while maintaining the exceptional salt-rejection performance for Na<ce:inf loc=\"post\">2</ce:inf>SO<ce:inf loc=\"post\">4</ce:inf> (&gt;97.0%). This high selectivity persisted even under challenging conditions of elevated salt concentration (8.0<ce:hsp sp=\"0.25\"></ce:hsp>g/L) and operating pressure (8.0<ce:hsp sp=\"0.25\"></ce:hsp>bar). The membrane exhibited robust rejection of various dyes (&gt;96%), sustained stability, and potent antifouling (BSA, FRR 89%) and antibacterial (&gt;99.97%) properties. Collectively, this work offers a mechanistic basis for designing zwitterionic NF membranes with high permeability, selectivity, and fouling resistance for treating complex hazardous wastewater.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"17 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149291069","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
From manure to fertilizer in minutes: radical induced humification and decontamination 从粪肥到肥料在几分钟内:自由基诱导腐殖质化和去污
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-10-29 DOI: 10.1016/j.jhazmat.2026.144072
Tao Zhang, Yanping Zhu, Pengjin Zhu, Junxiang Yang, Kaili Li, Yajuan Li, Yongle Yu, Cun Jiang, Guangpeng Wang, Xiuping Zhan, Chunhuo Zhou, Xin Yin, Guorong Ni, Naiqin Zhong, Pan Zhao, Shihu Shu, Dongfang Wang, Dongqing Cai
Global livestock/poultry manure output (approximately 13 billion tons/year) poses a major sustainability challenge. Conventional recycling via composting and anaerobic digestion after solid-liquid separation is slow (20-60 d) and inefficient at removing pollutants (i.e. pathogens, antibiotics, and heavy metals). This study develops a minute-scale, one-step process using microwave and FeSO₄ to activate persulfate, generating radicals that rapidly convert chicken manure into a fertilizer rich in fulvic-like acids (41.7wt% on a dry-product basis) and nutrients, including K (a primary nutrient) and Fe (a micronutrient). It simultaneously inactivates culturable bacteria, achieves approximately 99% removal of the parent antibiotics, reduces the combined acid-extractable and reducible fractions of Cd, Cu, and As by approximately 90%, and reduces odors (>97%). Carbon and nitrogen losses, calculated on an absolute-mass basis, were 15.6% and 12.6%, respectively. In a 21-day pot experiment, the fertilizer increased the fresh biomass of pak choi seedlings by 214.3% compared with the unamended soil control (Blank), while increasing soil total potassium and available nitrogen and potassium. This process shows cost (201 RMB/t wet CMPFM) advantage compared with composting, offering an efficient green alternative for manure recycling and circular agriculture.
全球畜禽粪便产量(约130亿吨/年)对可持续性构成重大挑战。固液分离后通过堆肥和厌氧消化进行的传统回收很慢(20-60天),而且在去除污染物(即病原体、抗生素和重金属)方面效率低下。本研究开发了一种分分钟规模的一步工艺,使用微波和FeSO₄来激活过硫酸盐,产生自由基,迅速将鸡粪转化为富含黄腐酸的肥料(在干品基础上为41.7wt%)和营养物质,包括K(主要营养素)和Fe(微量营养素)。它同时灭活可培养的细菌,达到约99%的母体抗生素去除率,将Cd, Cu和As的酸萃取和可还原部分减少约90%,并减少异味(97%)。以绝对质量为基础计算的碳和氮损失分别为15.6%和12.6%。在21 d盆栽试验中,与未施用土壤对照(空白)相比,施用有机肥使小白菜幼苗的新鲜生物量增加了214.3%,土壤全钾和速效氮、钾均有所增加。与堆肥相比,该工艺具有成本(201元/吨)的优势,为粪肥循环利用和循环农业提供了高效的绿色替代方案。
{"title":"From manure to fertilizer in minutes: radical induced humification and decontamination","authors":"Tao Zhang, Yanping Zhu, Pengjin Zhu, Junxiang Yang, Kaili Li, Yajuan Li, Yongle Yu, Cun Jiang, Guangpeng Wang, Xiuping Zhan, Chunhuo Zhou, Xin Yin, Guorong Ni, Naiqin Zhong, Pan Zhao, Shihu Shu, Dongfang Wang, Dongqing Cai","doi":"10.1016/j.jhazmat.2026.144072","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2026.144072","url":null,"abstract":"Global livestock/poultry manure output (approximately 13 billion tons/year) poses a major sustainability challenge. Conventional recycling via composting and anaerobic digestion after solid-liquid separation is slow (20-60 d) and inefficient at removing pollutants (i.e. pathogens, antibiotics, and heavy metals). This study develops a minute-scale, one-step process using microwave and FeSO₄ to activate persulfate, generating radicals that rapidly convert chicken manure into a fertilizer rich in fulvic-like acids (41.7<ce:hsp sp=\"0.25\"></ce:hsp>wt% on a dry-product basis) and nutrients, including K (a primary nutrient) and Fe (a micronutrient). It simultaneously inactivates culturable bacteria, achieves approximately 99% removal of the parent antibiotics, reduces the combined acid-extractable and reducible fractions of Cd, Cu, and As by approximately 90%, and reduces odors (&gt;97%). Carbon and nitrogen losses, calculated on an absolute-mass basis, were 15.6% and 12.6%, respectively. In a 21-day pot experiment, the fertilizer increased the fresh biomass of pak choi seedlings by 214.3% compared with the unamended soil control (Blank), while increasing soil total potassium and available nitrogen and potassium. This process shows cost (201 RMB/t wet CMPFM) advantage compared with composting, offering an efficient green alternative for manure recycling and circular agriculture.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"8 3 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149291065","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
Econazole prevents the conjugative transfer of plasmid-borne last-line antibiotic resistance genes Econazole可阻止质粒携带的最后一线抗生素耐药基因的结合转移
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-10-29 DOI: 10.1016/j.jhazmat.2026.144069
Hongye Hu, Ning Dong, Chunli Li, Guangfen Zhang, Yuanyuan Li, Yunbing Li, Xiaofan Li, Xiangkun Zeng, Jiayi You, Lili Huang, Ruichao Li, Mi Zhou, Sheng Chen, Shuyan Wu, Chen Xu
The global dissemination of antimicrobial resistance genes (ARGs) via plasmid-mediated conjugative transfer severely compromises the efficacy of last-resort antibiotics. Inhibiting this horizontal gene transfer represents a promising strategy to treat multidrug-resistant infections. In this study, we identified the FDA-approved antifungal agent Econazole (Econ) as a potent conjugation inhibitor. Conjugation assays with clinically relevant plasmids carrying mcr, blaNDM, blaKPC-2, tet(X4), or tmexCD1-toprJ1 showed that Econ inhibited transfer at 4–128μg/ml without affecting bacterial growth, reducing mcr-1 plasmid conjugation by approximately 33-fold at 128μg/ml. Mechanistically, membrane potential, ATP, and qRT-PCR analyses revealed that Econ dissipates the proton motive force and depletes ATP levels, impairing the energy-dependent type IV secretion system, with virB11 downregulated by 3- to 25-fold in the donor. Concurrently, Econ interferes with plasmid processing and attenuates the accumulation of single-stranded DNA, which consequently suppresses the SOS response in the recipient strain. Collectively, these findings elucidate the molecular mechanisms underlying the broad-spectrum inhibitory effect of Econ on conjugation, highlighting its translational potential for combating the dissemination of ARGs.
抗菌素耐药基因(ARGs)通过质粒介导的偶联转移在全球传播,严重损害了最后手段抗生素的疗效。抑制这种水平基因转移是治疗耐多药感染的一种有希望的策略。在这项研究中,我们发现fda批准的抗真菌药物Econazole (Econ)是一种有效的偶联抑制剂。与携带mcr、blaNDM、blaKPC-2、tet(X4)或tmexCD1-toprJ1的临床相关质粒的结合实验显示,Econ在4-128μg /ml浓度下抑制转移而不影响细菌生长,在128μg/ml浓度下使mcr-1质粒的结合率降低了约33倍。从机制上讲,膜电位、ATP和qRT-PCR分析显示,Econ耗散质子动力,消耗ATP水平,损害能量依赖性IV型分泌系统,在供体中virB11下调3- 25倍。同时,Econ干扰质粒加工并减弱单链DNA的积累,从而抑制受体菌株的SOS反应。总的来说,这些发现阐明了Econ对偶联的广谱抑制作用的分子机制,突出了其在对抗ARGs传播方面的转化潜力。
{"title":"Econazole prevents the conjugative transfer of plasmid-borne last-line antibiotic resistance genes","authors":"Hongye Hu, Ning Dong, Chunli Li, Guangfen Zhang, Yuanyuan Li, Yunbing Li, Xiaofan Li, Xiangkun Zeng, Jiayi You, Lili Huang, Ruichao Li, Mi Zhou, Sheng Chen, Shuyan Wu, Chen Xu","doi":"10.1016/j.jhazmat.2026.144069","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2026.144069","url":null,"abstract":"The global dissemination of antimicrobial resistance genes (ARGs) via plasmid-mediated conjugative transfer severely compromises the efficacy of last-resort antibiotics. Inhibiting this horizontal gene transfer represents a promising strategy to treat multidrug-resistant infections. In this study, we identified the FDA-approved antifungal agent Econazole (Econ) as a potent conjugation inhibitor. Conjugation assays with clinically relevant plasmids carrying <ce:italic>mcr</ce:italic>, <ce:italic>bla</ce:italic><ce:inf loc=\"post\">NDM</ce:inf>, <ce:italic>bla</ce:italic><ce:inf loc=\"post\">KPC-2</ce:inf>, <ce:italic>tet</ce:italic>(X4), or <ce:italic>tmexCD1-toprJ1</ce:italic> showed that Econ inhibited transfer at 4–128<ce:hsp sp=\"0.25\"></ce:hsp>μg/ml without affecting bacterial growth, reducing mcr-1 plasmid conjugation by approximately 33-fold at 128<ce:hsp sp=\"0.25\"></ce:hsp>μg/ml. Mechanistically, membrane potential, ATP, and qRT-PCR analyses revealed that Econ dissipates the proton motive force and depletes ATP levels, impairing the energy-dependent type IV secretion system, with <ce:italic>virB11</ce:italic> downregulated by 3- to 25-fold in the donor. Concurrently, Econ interferes with plasmid processing and attenuates the accumulation of single-stranded DNA, which consequently suppresses the SOS response in the recipient strain. Collectively, these findings elucidate the molecular mechanisms underlying the broad-spectrum inhibitory effect of Econ on conjugation, highlighting its translational potential for combating the dissemination of ARGs.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"11 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149291067","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
Simultaneous nutrient and PAH removal from municipal secondary effluent in pilot-scale open algal raceway ponds: Effects of hydraulic retention time and multi-trophic microbial succession 在中试开放藻槽池中同时去除城市二级污水中的营养物和多环芳烃:水力停留时间和多营养微生物演替的影响
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-10-29 DOI: 10.1016/j.jhazmat.2026.144074
Yanyan Yang, Ronghao Qiao, Chao Chang, Songqi Yang, Ming Li
Algal raceway ponds (ARPs) are considered one of the most promising technologies for the advanced treatment of wastewater treatment plant (WWTP) effluents. In this study, three parallel pilot-scale open ARPs, each assigned to one hydraulic retention time (HRT, 2, 3, or 4 d), were continuously operated for 52 d to assess nutrient and PAH removal, PAH partitioning, and microbial community succession. The 3-d system provided the most favorable observed balance between pond biomass accumulation and pollutant removal, with the highest mean pond biomass concentration (704mgL-1 (dw)) and mean removal efficiencies of 86.52%, 95.18%, 67.74%, 91.81%, and 73.68% for TN, TP, NH4+-N, NO3−-N, and Σ16PAH, respectively. Daily biomass harvesting was highest at 2 d (14.9gm-2 d-1 (dw)). At the 3-d HRT, the mean removal efficiencies of low-molecular-weight (LMW) and high-molecular-weight (HMW) PAHs were 74.39% and 69.61%, respectively. Distinct microbial assemblages developed in the ARPs, with Golenkinia predominating among microalgal genera, Pseudomonadota among bacterial phyla, and Cercozoa among protozoan phyla. Exploratory association analyses revealed that LMW-PAH removal showed positive directional relationships with OD680 and microalgal diversity, whereas HMW-PAH removal showed predominantly negative relationships with physiological, nutrient-removal, and community indicators. Phase-distribution analysis further showed that HMW-PAHs were enriched in harvested biomass and that logKd increased with logKow. Aqueous BaP-equivalent concentrations were lower in the effluents than in the influent, and incremental lifetime cancer risk estimates for harvested biomass were below 10-6 under the specified adult incidental-ingestion scenario. These findings support the engineering application of open ARP systems for advanced treatment of WWTP effluent.
藻槽池(ARPs)被认为是污水处理厂(WWTP)出水深度处理中最有前途的技术之一。在这项研究中,三个平行的中试规模的开放式ARPs,每个分配一个水力保留时间(HRT, 2,3或4 d),连续运行52天,以评估营养物质和多环芳烃的去除,多环芳烃的分配和微生物群落演替。三维系统在池塘生物量积累和污染物去除之间提供了最有利的平衡,平均池塘生物量浓度最高(704mgL-1 (dw)),对TN、TP、NH4+-N、NO3−-N和Σ16PAH的平均去除效率分别为86.52%、95.18%、67.74%、91.81%和73.68%。日生物量收获量在第2 d最高(14.9gm-2 d-1 (dw))。在3-d HRT下,低分子量(LMW)和高分子量(HMW) PAHs的平均去除率分别为74.39%和69.61%。在ARPs中形成了不同的微生物组合,在微藻属中占主导地位的是戈伦基尼菌,在细菌门中占主导地位的是假单胞菌,在原生动物门中占主导地位的是尾虫。探索性关联分析显示,低分子量pah去除率与OD680和微藻多样性呈正向关系,而低分子量pah去除率与生理、营养物去除率和群落指标呈显著负相关。相分布分析进一步表明,高分子量多环芳烃在收获生物量中富集,且logKd随logKow的增加而增加。出水水中的bap当量浓度低于进水,在特定的成人偶然摄入情景下,收获生物量的增量终生癌症风险估计值低于10-6。这些发现支持了开放式ARP系统在污水处理厂出水深度处理中的工程应用。
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引用次数: 0
Engineering FAST-PETase with Enhanced Catalytic Efficiency and Acidic Adaptability for Sustainable PET Waste Recycling 具有增强催化效率和酸性适应性的工程FAST-PETase用于PET废物的可持续回收
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-10-29 DOI: 10.1016/j.jhazmat.2026.144073
Haiquan Yang, Yiru Liu, Zhixing Shen, Yu Cao, Wei Shen, Yuanyuan Xia, Li Zhou, Xianzhong Chen
This study presented a comprehensive protein engineering strategy to enhance the catalytic efficiency and environmental adaptability of FAST-PETase for PET plastic degradation. Through systematic site-directed mutagenesis of key basic residues (Arg84, Arg117, and Lys227) surrounding the active site, we identified R84D as the optimal single mutant, exhibiting 2.1-fold higher activity than FAST-PETase. Iterative saturation mutagenesis at 19 targeted positions yielded the quadruple mutant R84D/A203T/S230K/E198Q, demonstrating superior kinetic parameters: 3.3-fold higher catalytic efficiency (kcat/Km = 10.8L·mmol-1·min-1) and significantly improved substrate affinity (Km = 72.6mM) at acidic conditions. Structural characterization revealed this mutant’s optimized active site geometry, featuring enhanced hydrogen bonding and hydrophobic interactions. It exhibited broad pH adaptability (maintaining >80% activity at pH 7.59.0) with a 0.5-unit acidic shift in optimal pH (7.5 vs wild-type’s 8.0), while retaining thermal stability up to 50°C. Molecular dynamics simulations confirmed the mutant’s enhanced structural rigidity, with 3050% lower RMSD values compared to FAST-PETase. When tested in a two-module reactor system, the quintuple mutant R84D/A203T/S230K/E198Q/S239V enabled efficient PET conversion to TPA, achieving a space-time conversion rate of 3.51g·(L·h)-1. These results demonstrated its practical potential for industrial application. It established an effective framework for engineering plastic-degrading enzymes with enhanced performance under industrially relevant conditions.
为了提高FAST-PETase对PET塑料降解的催化效率和环境适应性,本研究提出了一种综合的蛋白质工程策略。通过对活性位点周围的关键碱基(Arg84、Arg117和Lys227)进行系统的定点诱变,我们发现R84D是最佳的单突变体,其活性比FAST-PETase高2.1倍。在19个目标位置进行迭代饱和诱变,获得了四重突变体R84D/A203T/S230K/E198Q,具有较好的动力学参数:催化效率提高3.3倍(kcat/Km = 10.8L·mmol-1·min-1),在酸性条件下显著提高了底物亲和力(Km = 72.6mM)。结构表征揭示了该突变体优化的活性位点几何形状,具有增强的氢键和疏水相互作用。它表现出广泛的pH适应性(在pH值7.59.0时保持80%的活性),在最佳pH值(7.5 vs野生型8.0)下酸移0.5个单位,同时保持高达50°C的热稳定性。分子动力学模拟证实了该突变体的结构刚性增强,与FAST-PETase相比RMSD值降低了3050%。在双模块反应器系统中进行测试时,五重突变体R84D/A203T/S230K/E198Q/S239V使PET高效转化为TPA,实现了3.51g·(L·h)-1的时空转化率。这些结果表明了它在工业应用中的实际潜力。它为工程塑料降解酶在工业相关条件下提高性能建立了一个有效的框架。
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引用次数: 0
The C-terminal Fragment of COL1A1 Protects Mammalian Testicular BTB Integrity by Competitively Inhibiting Cd-Induced Activation of the TGFβ-SMAD2/3-MMP9 Pathway COL1A1的c端片段通过竞争性抑制cd诱导的TGFβ-SMAD2/3-MMP9通路的激活来保护哺乳动物睾丸BTB的完整性
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-10-29 DOI: 10.1016/j.jhazmat.2026.144054
Hao Xiong, Jialian Li, Anna Wu, Xinpeng Yang, Wenning Xu, Shang Wu, Shiqin Zhou, Gaogui Chen, Dake Chen, Jinhua Tang, Fenge Li
Cadmium (Cd), a heavy metal pollutant, impairs male reproductive health by disrupting the blood-testis barrier (BTB) and inducing testicular injury in mammals. Collagen type I alpha 1 chain (COL1A1) and its bioactive fragments are essential for maintaining BTB integrity and seminiferous tubule structure. However, whether COL1A1 and its bioactive fragments can modulate Cd-induced BTB injury remains largely unknown. In this study, proteomic analysis showed that downregulated proteins including COL1A1 were mainly enriched in collagen-containing extracellular matrix pathway in boars with low quality semen. COL1A1 generates an approximately 25kDa bioactive fragment termed C1158/59. Overexpression of C1158/59 in primary mouse Sertoli cells and testes mitigated Cd-induced BTB damage by restoring the expression and localization of BTB-associated proteins, as well as the organization of F-actin and α-tubulin cytoskeletons in Sertoli cells. Mechanistically, C1158/59 competitively inhibited the binding of latent TGFβ to ITGB1, suppressing Cd-induced activation of the TGFβ-SMAD2/3 signaling pathway and subsequent MMP9 upregulation, ultimately preventing BTB structural degradation. Collectively, these findings demonstrate a critical protective role of the COL1A1-derived fragment C1158/59 against Cd-induced structural and functional impairment of the testicular BTB, providing new insights into the regulatory functions of bioactive fragments in preserving BTB structural integrity against environmental toxicant-induced testicular injury.
镉(Cd)是一种重金属污染物,通过破坏哺乳动物血睾丸屏障(BTB)和引起睾丸损伤而损害男性生殖健康。I型胶原α - 1链(COL1A1)及其生物活性片段对维持BTB完整性和精管结构至关重要。然而,COL1A1及其生物活性片段是否能调节cd诱导的BTB损伤仍是未知的。蛋白质组学分析表明,低品质精液公猪体内COL1A1等下调蛋白主要富集于含胶原细胞外基质通路。COL1A1产生约25kDa的生物活性片段,称为C1158/59。C1158/59在原代小鼠支持细胞和睾丸中过表达,通过恢复支持细胞中BTB相关蛋白的表达和定位,以及F-actin和α-微管蛋白细胞骨架的组织,减轻cd诱导的BTB损伤。机制上,C1158/59竞争性地抑制潜伏的TGFβ与ITGB1的结合,抑制cd诱导的TGFβ- smad2 /3信号通路的激活和随后的MMP9上调,最终阻止BTB结构降解。总之,这些发现证明了col1a1衍生片段C1158/59对cd诱导的睾丸BTB结构和功能损伤的关键保护作用,为生物活性片段在保护BTB结构完整性免受环境毒物诱导的睾丸损伤方面的调节功能提供了新的见解。
{"title":"The C-terminal Fragment of COL1A1 Protects Mammalian Testicular BTB Integrity by Competitively Inhibiting Cd-Induced Activation of the TGFβ-SMAD2/3-MMP9 Pathway","authors":"Hao Xiong, Jialian Li, Anna Wu, Xinpeng Yang, Wenning Xu, Shang Wu, Shiqin Zhou, Gaogui Chen, Dake Chen, Jinhua Tang, Fenge Li","doi":"10.1016/j.jhazmat.2026.144054","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2026.144054","url":null,"abstract":"Cadmium (Cd), a heavy metal pollutant, impairs male reproductive health by disrupting the blood-testis barrier (BTB) and inducing testicular injury in mammals. Collagen type I alpha 1 chain (COL1A1) and its bioactive fragments are essential for maintaining BTB integrity and seminiferous tubule structure. However, whether COL1A1 and its bioactive fragments can modulate Cd-induced BTB injury remains largely unknown. In this study, proteomic analysis showed that downregulated proteins including COL1A1 were mainly enriched in collagen-containing extracellular matrix pathway in boars with low quality semen. COL1A1 generates an approximately 25<ce:hsp sp=\"0.25\"></ce:hsp>kDa bioactive fragment termed C1158/59. Overexpression of C1158/59 in primary mouse Sertoli cells and testes mitigated Cd-induced BTB damage by restoring the expression and localization of BTB-associated proteins, as well as the organization of F-actin and α-tubulin cytoskeletons in Sertoli cells. Mechanistically, C1158/59 competitively inhibited the binding of latent TGFβ to ITGB1, suppressing Cd-induced activation of the TGFβ-SMAD2/3 signaling pathway and subsequent MMP9 upregulation, ultimately preventing BTB structural degradation. Collectively, these findings demonstrate a critical protective role of the COL1A1-derived fragment C1158/59 against Cd-induced structural and functional impairment of the testicular BTB, providing new insights into the regulatory functions of bioactive fragments in preserving BTB structural integrity against environmental toxicant-induced testicular injury.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"21 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149291068","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
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Journal of Hazardous Materials
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