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How Rhodococcus ruber accelerated biodegradation of benzophenone-3 红葡萄球菌如何加速二苯甲酮-3 的生物降解
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-18 DOI: 10.1016/j.jhazmat.2024.136566
Fei Liu, Yue Ma, Wenxuan Li, Jue Cai, Haiyun Zhang, Fu Chen, Yongming Zhang, Bruce E. Rittmann
Benzophenone-3 (2-hydroxy-4-methoxybenzophenone, BP-3) poses risks to human health and natural ecosystems, and means to improve its biodegradation are necessary. When a small mass of Rhodococcus ruber, isolated from BP-3-acclimated biomass, was bioaugmented into the acclimated biomass, BP-3 removal was accelerated by 120%. The first step of BP-3 biodegradation generates either 2,5-dihydroxy-4-methoxybenzophenone (5-OH-BP-3) or benzophenone-1 (2,4-dihydoxybenzophenone, BP-1). BP-1 is generated by sequential demethylation, hydroxylation, and dehydrogenation reactions, while 5-OH-BP-3 is generated by one mono-oxygenation reaction. Of the two intermediates, 5-OH-BP-3 exhibited stronger inhibition than BP-1 or the original BP-3. Gene-completion mapping showed that R. ruber contains genes for demethylase, hydrolase, dehydrogenase, and mono-oxygenase reaction, which means that R. ruber could generate the less-toxic BP-1. Thus, bioaugmentation of R. ruber into BP-3-acclimated biomass eliminated the accumulation of 5-OH-BP-3 and, consequently, accelerated of BP-3 biodegradation via BP-1.
二苯甲酮-3(2-羟基-4-甲氧基二苯甲酮,BP-3)对人类健康和自然生态系统构成风险,因此有必要改善其生物降解。将从 BP-3 适应生物质中分离出的少量红球菌(Rhodococcus ruber)生物增殖到适应生物质中,BP-3 的去除速度加快了 120%。BP-3 生物降解的第一步是生成 2,5-二羟基-4-甲氧基二苯甲酮(5-OH-BP-3)或二苯甲酮-1(2,4-二羟基二苯甲酮,BP-1)。BP-1 是通过连续的脱甲基、羟基和脱氢反应生成的,而 5-OH-BP-3 则是通过一个单氧反应生成的。在这两种中间产物中,5-OH-BP-3 比 BP-1 或原始 BP-3 表现出更强的抑制作用。基因补全图谱显示,R. ruber 含有去甲基化酶、水解酶、脱氢酶和单加氧酶反应的基因,这意味着 R. ruber 可以生成毒性较低的 BP-1。因此,将 R. ruber 生物增殖到 BP-3 适应的生物质中,可消除 5-OH-BP-3 的积累,从而通过 BP-1 加速 BP-3 的生物降解。
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引用次数: 0
Exogenous additives reshape the microbiome and promote the reduction of resistome in co-composting of pig manure and mushroom residue 外源添加剂重塑微生物组,促进猪粪和蘑菇渣共堆肥中抗微生物组的减少
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-18 DOI: 10.1016/j.jhazmat.2024.136544
Li Zhang, Lan Jiang, Wenjing Yan, Hanxiang Tao, Chengcheng Yao, Lu An, Yifan Sun, Ting Hu, Wei Sun, Xun Qian, Jie Gu
Comprehensive understanding of the microbiome and resistome evolution in compost is crucial for guaranteeing the safety of organic fertilizers. Current studies using different composting systems and sequencing technologies have yielded varying conclusions on the efficacy of exogenous additives (EAs) in reducing antibiotic resistance genes (ARGs) in compost. This study employed metagenomics to investigate the impact of various EAs on microbial communities, ARGs, their coexistence with mobile genetic elements (MGEs), and ARG hosts in co-composting. Our results demonstrated that EAs significantly reshaped the microbial communities and facilitated a notable reduction in total ARG abundance and diversity, primarily by decreasing core ARGs. Cooperative rather than antagonistic relationships among bacteria. The RA changes in total ARGs are mainly caused by a decrease in the prevalence of core ARGs. Furthermore, EAs showed significant efficacy in reducing clinical ARGs, including cfxA, tetX1, cfxA6, vanA, and aac (6')-Ib', with diatomite (5%) and zeolite (5%) being the most effective. The effect of EAs on ARGs and microbial community assembly were stochastic processes. Composting stage and EAs jointly reduced the association between ARGs and MGEs in the composting system. The reduction of ARGs attributed to a decreased abundance of potential pathogenic ARG-associated hosts and diminished associations with MGEs. In conclusion, EAs present a straightforward and effective approach for promoting ARGs reduction in compost, offering crucial insights for assessing the environmental risks associated with the release of agricultural ARGs.
全面了解堆肥中的微生物组和抗药性基因组的进化对于保证有机肥料的安全性至关重要。目前使用不同堆肥系统和测序技术进行的研究对外源添加剂(EAs)在减少堆肥中抗生素抗性基因(ARGs)方面的功效得出了不同的结论。本研究采用元基因组学方法研究了各种 EAs 对微生物群落、ARGs、它们与移动遗传因子(MGEs)共存以及共堆肥中 ARGs 宿主的影响。我们的研究结果表明,EA 显著重塑了微生物群落,并主要通过减少核心 ARG,促进了 ARG 总丰度和多样性的显著降低。细菌之间是合作关系而非拮抗关系。ARGs 总量的 RA 变化主要是由核心 ARGs 的减少引起的。此外,EAs 对减少临床 ARGs(包括 cfxA、tetX1、cfxA6、vanA 和 aac (6')-Ib')有明显的效果,其中硅藻土(5%)和沸石(5%)的效果最好。EA对ARGs和微生物群落组合的影响是随机过程。堆肥阶段和 EAs 共同减少了堆肥系统中 ARGs 和 MGEs 之间的关联。ARGs 的减少归因于潜在致病性 ARG 相关宿主数量的减少以及与 MGEs 联系的减少。总之,EAs 是促进减少堆肥中 ARGs 的一种直接而有效的方法,为评估与农业 ARGs 释放有关的环境风险提供了重要依据。
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引用次数: 0
Activated electrolytic manganese residue-based environmental materials for mine remediation: Performance and mechanism 基于活性电解锰渣的矿山修复环境材料:性能和机理
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-18 DOI: 10.1016/j.jhazmat.2024.136560
Tianyu Zeng, Size Xue, Shiyu Zhuang, Xian Zhou, Haobo Hou, Bo-Tao Huang, Jirong Lan
To address the environmental hazards of electrolytic manganese residue (EMR) accumulation and the urgent need for ecological restoration in mining areas, we developed an innovative method for creating pit restoration materials (S-EMRs) using alkaline-excited EMR via mechanical ball milling. Black liquid (BL) was used as a base exciter and EMR as the precursor. With a BL dosage of 35%, alumina as the milling medium, a speed of 500 rpm, and milling for 20–35 min, we achieved an S-EMR compressive strength of approximately 30 MPa after 14 d—six times higher than that in conventional cement curing (C-EMR). This method also stabilized contaminants such as Mn and NH4+ by over 10-fold. The self-cementation and formation mechanisms of the S-EMR were clarified through chemical characterization and geochemical modeling. Over 3 y of monitoring and plant experiments have shown that S-EMR ensured the long-term stability and ecological restoration of mining areas. Remarkably, it enhanced microbial diversity and biophilicity, improving tomato seed germination by over 90% compared with that in control. This study presents a sustainable and innovative solution for the green cycle rehabilitation of Mn mining areas with significant potential for engineering applications.
针对电解锰残渣(EMR)积累对环境造成的危害和矿区生态恢复的迫切需要,我们开发了一种创新方法,利用碱激发的 EMR 通过机械球磨制造矿坑恢复材料(S-EMR)。黑液(BL)用作基础激发剂,EMR 用作前驱体。黑液用量为 35%,氧化铝作为研磨介质,转速为 500 rpm,研磨时间为 20-35 min,14 d 后,我们获得了约 30 MPa 的 S-EMR 抗压强度,是传统水泥固化法(C-EMR)的六倍。这种方法还能使锰和 NH4+ 等污染物的稳定性提高 10 倍以上。通过化学特征描述和地球化学建模,阐明了 S-EMR 的自固化和形成机制。超过 3 年的监测和植物实验表明,S-EMR 确保了矿区的长期稳定和生态恢复。值得注意的是,它提高了微生物多样性和亲生物性,与对照组相比,番茄种子发芽率提高了 90% 以上。这项研究为锰矿开采区的绿色循环恢复提供了一种可持续的创新解决方案,具有巨大的工程应用潜力。
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引用次数: 0
Microplastic in bivalves of an urbanized Brazilian estuary: human modification, population density and vegetation influence 巴西城市化河口双壳类动物体内的微塑料:人类活动、人口密度和植被的影响
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-17 DOI: 10.1016/j.jhazmat.2024.136546
Victor Vasques Ribeiro, Nuria Casado-Coy, Danilo Freitas Rangel, Carlos Sanz-Lazaro, Ítalo Braga Castro
Microplastics (MPs) global ubiquitously affects particularly coastal regions under significant anthropogenic pressures, where there are limited monitoring efforts. Bivalves are valuable sentinels of MPs contamination. This investigation determined MP contamination in oysters, clams, and mussels at Santos-São Vicente, a heavily urbanized estuary in Brazil, focusing on socio-environmental predictors, spatial distribution, and interspecies variations. Elevated MPs levels were linked to higher human modification (β = 0.5747, p = 0.0223) and reduced population density (β = -8.918e-06, p = 0.0443), regardless of vegetation cover (p > 0.05). Such a negative connection between population density and MP contamination occurred due to the significant presence of industrial and port activities, leading to high MP discharges despite a low population. The simultaneous presence of the three species at specific sites is an intrinsic limitation for broad spatial studies, depending on their environmental availability. Despite higher concentrations in clams, mussels and oysters also exhibited spatial variations in MP concentrations, serving as suitable sentinels. The central and left segments of the estuary displayed elevated MP concentrations, consistent with a well-known contamination gradient. Clams accumulated more MPs (1.97 ± 1.37 [0.00 – 5.55] particles.g-1) than mussels (0.72 ± 1.07 [0.00 – 7.74] particles.g-1) and oysters (0.70 ± 1.03 [0.00 – 7.70] particles.g-1), suggesting higher bioavailability in sediments than the water column. MPs found across all species were predominantly smaller (<1,000 µm), fragments or fibers, and colorless. These discoveries lay a groundwork for prospective global investigations by linking MPs concentrations to socio-environmental predictors, contributing to the development of local mitigation measures and global discussions.
微塑料(MPs)对全球的影响无处不在,尤其是在人为压力巨大的沿海地区,而这些地区的监测工作却十分有限。双壳类动物是微塑料污染的重要哨兵。这项调查确定了巴西桑托斯-圣维森特(Santos-São Vicente)的牡蛎、蛤蜊和贻贝中的多溴联苯醚污染情况,重点关注社会环境预测因素、空间分布和物种间变化。MPs水平的升高与较高的人为改造(β = 0.5747,p = 0.0223)和人口密度的降低(β = -8.918e-06,p = 0.0443)有关,与植被覆盖度无关(p > 0.05)。人口密度与 MP 污染之间的负相关是由于工业和港口活动的大量存在,导致尽管人口较少,但 MP 排放量较高。这三个物种同时出现在特定地点,对广泛的空间研究来说是一个内在的限制,这取决于它们的环境可用性。尽管蛤类的 MP 浓度较高,但贻贝和牡蛎的 MP 浓度也表现出空间变化,可作为合适的哨兵。河口中部和左部的 MP 浓度较高,与众所周知的污染梯度一致。与贻贝(0.72 ± 1.07 [0.00 - 7.74] 颗粒.g-1)和牡蛎(0.70 ± 1.03 [0.00 - 7.70] 颗粒.g-1)相比,蛤蜊积累了更多的 MPs(1.97 ± 1.37 [0.00 - 5.55] 颗粒.g-1),这表明沉积物中的生物利用率高于水体。在所有物种中发现的 MPs 主要较小(1,000 µm)、碎片或纤维,且无色。这些发现通过将 MPs 浓度与社会环境预测因素联系起来,为未来的全球调查奠定了基础,有助于制定当地的缓解措施和开展全球讨论。
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引用次数: 0
Pollutant-free pyrolysis strategy for direct upgrading of cathode materials from spent lithium-ion batteries 从废旧锂离子电池中直接升级正极材料的无污染热解战略
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-17 DOI: 10.1016/j.jhazmat.2024.136553
Pengwei Li, Shaohua Luo, Guodong Hao, Kuo Sun, Qiuyue Liu, Martin Møller, Deyong Wang, Peter Kjær Kristensen, Leonid Gurevich, Lars Rosgaard Jensen, Li Wang, Xiangming He
The recycling of lithium-ion batteries (LIBs) has been dogged by air pollutants containing fluoride (e.g. HF, PF5, POF3). Pyrolysis is a technique that can eliminate polyvinylidene fluoride (PVDF) from the cathode electrode sheets of spent LIBs, effectively separating the cathode material from the aluminum (Al) foil. Nonetheless, the HF gas generated during pyrolysis not only corrodes equipment but also presents serious environmental risks. To address this, a novel, eco-friendly strategy is introduced for the direct upgrading of cathode active materials (CAM). The strategy's cornerstone involves incorporating a minor amount of calcium into the original cathode material's coating, and it leverages mechanical stirring during the waste battery material separation process to ensure the electrode is fully detached from the current collector at a reduced temperature. The pyrolysis mechanism elucidates that fluorine-containing organic pollutants are converted into metal fluorides and deposited on the surface of cathode particles during aerobic pyrolysis, thereby improving the interfacial stability of lithium nickel cobalt manganese oxide (NCM) materials, reducing transition metal dissolution. This strategy not only eliminates the release of fluorine-containing organic pollutants during pyrolysis but also achieves direct regeneration of CAM. This work underscores the importance of the cathode materials' manufacturing process in facilitating the recycling of spent LIBs and provides an environmentally friendly and economically viable solution for the battery recycling industry.
锂离子电池(LIB)的回收利用一直受到含氟空气污染物(如 HF、PF5、POF3)的困扰。热解技术可以消除废锂离子电池阴极电极片上的聚偏二氟乙烯(PVDF),从而有效地将阴极材料与铝(Al)箔分离。然而,热解过程中产生的 HF 气体不仅会腐蚀设备,还会带来严重的环境风险。为了解决这个问题,我们引入了一种新颖、环保的阴极活性材料(CAM)直接升级策略。该策略的基石是在原始阴极材料涂层中加入少量钙,并利用废电池材料分离过程中的机械搅拌,确保电极在较低温度下与集流器完全分离。热解机理阐明了含氟有机污染物在有氧热解过程中转化为金属氟化物并沉积在阴极颗粒表面,从而提高了锂镍钴锰氧化物(NCM)材料的界面稳定性,减少了过渡金属的溶解。这一策略不仅消除了热解过程中含氟有机污染物的释放,还实现了 CAM 的直接再生。这项工作强调了阴极材料制造工艺在促进废 LIB 回收方面的重要性,并为电池回收行业提供了一种环保且经济可行的解决方案。
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引用次数: 0
Effect of microplastics concentration and size on pollutants removal and antibiotic resistance genes (ARGs) generation in constructed wetlands: a metagenomics insight 微塑料的浓度和大小对建构湿地污染物清除和抗生素耐药基因(ARGs)生成的影响:元基因组学的启示
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-17 DOI: 10.1016/j.jhazmat.2024.136555
Lin Liang, Weiliang Pan, Merui Mu, Lin Zhang, Xiangyu Yang, Ruina Zhang, Lianfeng Du, Xuan Guo
The accrual of microplastics (MPs) and antibiotics poses synergistic threats to the environment. This study systemically examined the effect of environmental-level (μg/L) MPs (90–110 μm) and nanoplastics (NPs, 700 nm) on constructed wetlands (CWs) treating oxytetracycline-contaminated wastewater via metagenomics analysis. Polystyrene (PS) MPs notably hindered the removal of nitrogen, phosphorus, and oxytetracycline, particularly at high level (1000 μg/L), with removal rates of 73.34%, 59.59%, and 99.34%, respectively. Among them, the removal of NH4+-N decreased the most in comparison to CK, at 15.26%. Antibiotic resistance genes (ARGs) copies/16S rRNA ranged from 0.26 to 0.42 in CWs, exceeding that found in rivers by a factor of 1.5 to 2.5 times. The relative abundance of multidrug resistance genes (mdtB, acrB, mexF, mdtC, and mexT) and tetracycline resistance genes (txtA, tetG, and tetP) exhibited a pronounced increase under MPs exposure, ranging from 0.06 to 0.14 and 0.01 to 0.08 copies/16S rRNA, respectively. Redundancy and network analyses emphasized robust associations among contaminant reduction, ARG abundance, and microbial community. Partial least squares path modeling indicated MPs exerted a more profound influence on pollutant removal (coefficient = 0.8194), microbial community (coefficient = 0.3358) and ARGs dissemination (coefficient = 0.6566) compared to NPs. MPs concentrations significantly affects pollutants removal and ARGs proliferation, and MPs with larger sizes amplified ARG dissemination. This research highlights the influence of MPs on CW-mediated wastewater treatment and ARGs accumulation, offering valuable insights for developing ecological wastewater treatment strategies tailored to multi-pollutant scenarios. These insights are fundamental in developing sustainable solutions to the adverse impacts of MPs on ecosystems.
微塑料(MPs)和抗生素的累积对环境构成了协同威胁。本研究通过元基因组学分析,系统研究了环境水平(μg/L)的MPs(90-110 μm)和纳米塑料(NPs,700 nm)对处理土霉素污染废水的人工湿地(CWs)的影响。聚苯乙烯(PS)多孔塑料明显阻碍了氮、磷和土霉素的去除,尤其是在高浓度(1000 μg/L)时,去除率分别为 73.34%、59.59% 和 99.34%。其中,与 CK 相比,NH4+-N 的去除率下降最多,为 15.26%。化武中的抗生素耐药基因(ARGs)拷贝数/16S rRNA 在 0.26 至 0.42 之间,是河流中的 1.5 至 2.5 倍。多药耐药基因(mdtB、acrB、mexF、mdtC 和 mexT)和四环素耐药基因(txtA、tetG 和 tetP)的相对丰度在 MPs 暴露下明显增加,分别为 0.06 至 0.14 和 0.01 至 0.08 个拷贝/16S rRNA。冗余和网络分析强调了污染物减少、ARG 丰度和微生物群落之间的密切联系。偏最小二乘法路径模型显示,与 NPs 相比,MPs 对污染物去除(系数 = 0.8194)、微生物群落(系数 = 0.3358)和 ARGs 传播(系数 = 0.6566)的影响更为深远。MPs 的浓度对污染物的去除和 ARGs 的增殖有明显影响,尺寸较大的 MPs 会扩大 ARGs 的传播。这项研究强调了 MPs 对以 CW 为媒介的废水处理和 ARGs 积累的影响,为开发适用于多污染物情况的生态废水处理策略提供了宝贵的见解。这些见解对于制定可持续的解决方案,解决 MPs 对生态系统的不利影响至关重要。
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引用次数: 0
Antibiotic resistance evolution driven synergistically by antibiotics and typical organic pollutants in antibiotic production wastewater 抗生素生产废水中抗生素和典型有机污染物协同驱动的抗生素耐药性进化
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-17 DOI: 10.1016/j.jhazmat.2024.136543
Sun Miao, Yanyan Zhang, Xin Yuan, Jiane Zuo
A major concern regarding the risk of antibiotic production wastewater (APW) for the transmission of antibiotic resistance (AR) stems from the residual antibiotics. However, APW also contains high concentrations of organic pollutants, many of which have severe biological toxicity and joint toxicity with antibiotics. The contribution of these organic pollutants to the development of AR in the APW treatment system is unknown. In this study, a wild-type Escherichia coli strain was exposed to six typical organic pollutants in APW individually and synergistically with the antibiotic ampicillin (AMP). Independent exposure to organic compounds had negligible effects on the evolution of AR, whereas they synergistically induced AR mutations and increased antibiotic persistence with AMP, especially the raw material d-p-hydroxyphenylglycine (DHPG), at relevant concentrations in APW. Combined exposure to 1–500 mg/L DHPG and 1 mg/L AMP synergistically increased the mutation frequencies against multiple antibiotics by up to 2928.9-fold in a dose–time pattern, and the combination index reached 445.7. Phenotypic and genotypic analyses revealed that the synergism between DHPG and AMP was associated with increased antibacterial activity, enhanced oxidative stress, and stimulation of efflux pump expression. Overall, our results highlight the elevated risk of AR induction caused by antibiotics and organic pollutants in APW.
抗生素生产废水(APW)传播抗生素耐药性(AR)的风险主要来自于残留的抗生素。然而,抗生素生产废水中还含有高浓度的有机污染物,其中许多都具有严重的生物毒性以及与抗生素的联合毒性。这些有机污染物对 APW 处理系统中 AR 的形成有多大影响尚不清楚。在本研究中,野生型大肠埃希氏菌株单独暴露于亚太地区污水处理系统中的六种典型有机污染物,并与抗生素氨苄西林(AMP)协同作用。单独暴露于有机化合物对 AR 的进化影响微乎其微,而在 APW 中的相关浓度下,它们与 AMP(尤其是原料 d-对羟基苯甘氨酸(DHPG))协同诱导 AR 突变并增加抗生素的持久性。在剂量-时间模式下,1-500 毫克/升 DHPG 和 1 毫克/升 AMP 的联合接触可协同增加抗多种抗生素的突变频率,最高可达 2928.9 倍,联合指数达到 445.7。表型和基因型分析表明,DHPG 和 AMP 的协同作用与抗菌活性增加、氧化应激增强和外排泵表达刺激有关。总之,我们的研究结果突显了抗生素和有机污染物在亚太水产养殖中诱导 AR 的风险升高。
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引用次数: 0
Mobilization of poly- and perfluoroalkyl substances (PFAS) from heterogeneous soils: Desorption by ethanol/xanthan gum mixture 从异质土壤中迁移多氟和全氟烷基物质(PFAS):乙醇/黄原胶混合物的解吸作用
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-17 DOI: 10.1016/j.jhazmat.2024.136496
Ali Batikh, Stéfan Colombano, Maxime Cochennec, Dorian Davarzani, Arnault Perrault, Julie Lions, Julien Grandclément, Dominique Guyonnet, Anne Togola, Clément Zornig, Nicolas Devau, Fabien Lion, Amir Alamooti, Sébastien Bristeau, Mohamed Djemil, Eric D. van Hullebusch
Remediating soils contaminated by per- and polyfluoroalkyl substances (PFAS) is a challenging task due to the unique properties of these compounds, such as variable solubility and resistance to degradation. In-situ soil flushing with solvents has been considered as a remediation technique for PFAS-contaminated soils. The use of non-Newtonian fluids, displaying variable viscosity depending on the applied shear rate, can offer certain advantages in improving the efficiency of the process, particularly in heterogeneous porous media. In this work, the efficacy of ethanol/xanthan mixture (XE) in the recovery of a mixture of perfluorooctane sulfonate (PFOS), perfluorooctanoic acid (PFOA), perfluorohexane sulfonate (PFHxS), and perfluorobutane sulfonate (PFBS) from soil has been tested at lab-scale. XE’s non-Newtonian behavior was examined through rheological measurements, confirming that ethanol did not affect xanthan gum’s (XG) shear-thinning behavior. The recovery of PFAS in batch-desorption exceeded 95% in ethanol, and 99% in XE, except for PFBS which reached 94%. 1D-column experiments revealed overshoots in PFAS breakthrough curves during ethanol and XE injection, due to over-solubilization. XE, (XG 0.05% w/w) could recover 99% PFOA, 98% PFBS, 97% PFHxS, and 92% PFOS. Numerical modeling successfully reproduces breakthrough curves for PFOA, PFHxS, and PFBS with the convection-dispersion-sorption equation and Langmuir sorption isotherm.
由于全氟烷基和多氟烷基物质(PFAS)具有独特的性质,例如溶解度和抗降解性各不相同,因此对这些化合物污染的土壤进行修复是一项具有挑战性的任务。使用溶剂原位冲洗土壤被认为是一种针对受 PFAS 污染的土壤的修复技术。非牛顿流体的粘度随剪切速率的变化而变化,使用非牛顿流体在提高工艺效率方面具有一定的优势,尤其是在异质多孔介质中。在这项工作中,在实验室规模下测试了乙醇/黄原胶混合物(XE)从土壤中回收全氟辛烷磺酸(PFOS)、全氟辛酸(PFOA)、全氟己烷磺酸(PFHxS)和全氟丁烷磺酸(PFBS)混合物的功效。通过流变学测量检验了 XE 的非牛顿行为,证实乙醇不会影响黄原胶 (XG) 的剪切稀化行为。在批量脱附过程中,除全氟辛烷磺酸(PFBS)的回收率达到 94% 外,其他全氟辛烷磺酸(PFAS)在乙醇中的回收率超过 95%,在 XE 中的回收率超过 99%。一维柱实验显示,在乙醇和 XE 注入过程中,由于过度溶解,PFAS 的突破曲线出现了过冲。XE (XG 0.05% w/w)可回收 99% 的 PFOA、98% 的 PFBS、97% 的 PFHxS 和 92% 的 PFOS。利用对流-分散-吸附方程和 Langmuir 吸附等温线建立的数值模型成功地再现了 PFOA、PFHxS 和 PFBS 的突破曲线。
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引用次数: 0
Practical Limits of Current Technologies in Removing Per- and Polyfluoroalkyl Substances from Fire Suppression Systems 从灭火系统中去除全氟和多氟烷基物质的现有技术的实际局限性
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-17 DOI: 10.1016/j.jhazmat.2024.136551
Dung Nguyen, Christopher Bellona, Adria Lau, John Stults, Hayley Andrews, David Jones, David Megson, Ian Ross
Several commercial products have been broadly marketed for their effectiveness in removing residual PFAS from AFFF-impacted fire suppression systems. However, a comprehensive assessment of their effectiveness in mitigating long-term PFAS rebound following the initial cleaning has not been reported. Herein, batch and flow-through experiments were conducted to interrogate the overall effectiveness of four different cleaning solutions in removing residual PFAS from AFFF-impacted stainless steel pipes from a fire suppression system. Advanced surface imaging techniques were also employed to correlate with bench-scale testing results and to provide insights into potential PFAS rebound mechanisms. Results presented herein demonstrate that complete removal of PFAS from AFFF-impacted fire suppression systems is extremely difficult to achieve for all four cleaning solutions examined in this study. The PFAS rebound behavior observed was likely attributable to PFAS supramolecular assemblies accumulating on the pipe surfaces. Because PFAS rebound following cleanout of AFFF-impacted fire suppression systems is likely inevitable, there needs to be an understanding of the practical limits to which impacted fire suppression system cleanout can be achieved. Improved insights into the dissolution mechanisms and the rate of dissolution of supramolecular formations will be key to improving PFAS decontamination processes and decontamination of materials/equipment impacted by AFFFs.
有几种商业产品因其能有效清除受 AFFF 影响的灭火系统中残留的 PFAS 而被广泛推广。然而,对这些产品在初步清洁后减轻全氟辛烷磺酸长期反弹的效果进行全面评估的报道却寥寥无几。在此,我们进行了批量和流动实验,以检验四种不同的清洁溶液在去除灭火系统中受 AFFF 影响的不锈钢管道中残留的 PFAS 方面的总体效果。此外,还采用了先进的表面成像技术,以便与台架试验结果进行关联,并深入了解潜在的 PFAS 反弹机制。本文介绍的结果表明,对于本研究中检测的所有四种清洁溶液来说,要完全清除受 AFFF 影响的灭火系统中的 PFAS 都非常困难。所观察到的 PFAS 反弹行为很可能是由于管道表面积累了 PFAS 超分子集合体。由于在清理受 AFFF 影响的灭火系统后,PFAS 反弹可能不可避免,因此需要了解受影响的灭火系统清理所能达到的实际极限。更好地了解超分子结构的溶解机制和溶解速度将是改进 PFAS 净化过程和净化受 AFFF 影响的材料/设备的关键。
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引用次数: 0
Scale-up construction of stable multifunctional hydrogel interfaces for large-scale purification of complex oil-water emulsions and oil recovery 为大规模净化复杂油水乳化液和采油大规模构建稳定的多功能水凝胶界面
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-17 DOI: 10.1016/j.jhazmat.2024.136552
Hui Qiao, Qile Zhao, Jie Li, Hang Lu, Jinfang Wu, Liting Yang, Yuxin Ma, Yue Yin, Fang Guo, Yiwen Wang, Wenbo Wang
Inspired by the multi-level structure of grass clumps in nature, a novel filter with plexiform-structured hydrogel interface was constructed using sepiolite-derived silica nanofiber (SiNF) as the supporter and crosslinked polyvinyl alcohol (cl-PVA) hydrogel as the coating. Experimental test, DFT and MD calculations have confirmed that the addition of SiNF can not only enhance oil-water separation efficiency, but also improve the stability of hydrogel coating. The hydrogel interface with excellent stability and superhydrophilic/underwater superoleophobicity can be manufactured on a large copper mesh (1 m × 1.2 m) to achieve large-scale production. The surface-engineered mesh (named cl-PVA/SiNF@Ag-Cu) can be assembled on a self-designed equipment for continuous purification of emulsion wastewater (processing capacity: 576.00 L/day), achieving a high separation efficiency of 99.7% for complex oily emulsion only under the action of gravity, and can simultaneously recover oils. After being treated under extreme conditions such as strong acid/alkali, high/low temperature (100°C, 200°C, and -18°C), high salt concentration, sandpaper wear, and long-term aging, the surface structure of cl-PVA/SiNF@Ag-Cu filter remains stable. The antifouling, antibacterial, and anticorrosion capabilities of the filter give it the potential for long-term and large-scale purification processes. Planting and breeding experiments have confirmed that purified water is harmless to animals and plants.
受自然界草团多层次结构的启发,研究人员以sepiolite衍生的二氧化硅纳米纤维(SiNF)为支撑体,以交联聚乙烯醇(cl-PVA)水凝胶为涂层,构建了一种具有丛状结构水凝胶界面的新型过滤器。实验测试、DFT 和 MD 计算证实,加入 SiNF 不仅能提高油水分离效率,还能改善水凝胶涂层的稳定性。在大型铜网(1 m × 1.2 m)上可制造出具有优异稳定性和超亲水性/水下超疏水性的水凝胶界面,从而实现大规模生产。这种表面工程网(名为 cl-PVA/SiNF@Ag-Cu)可装配在自行设计的设备上,用于连续净化乳化液废水(处理能力:576.00 升/天),仅在重力作用下就能实现对复杂含油乳化液高达 99.7% 的分离效率,并能同时回收油类。经过强酸/碱、高/低温(100°C、200°C 和 -18°C)、高盐浓度、砂纸磨损和长期老化等极端条件处理后,cl-PVA/SiNF@Ag-Cu 过滤器的表面结构仍然保持稳定。过滤器的防污、抗菌和防腐功能使其具备了长期和大规模净化过程的潜力。种植和养殖实验证实,净化后的水对动植物无害。
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引用次数: 0
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Journal of Hazardous Materials
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