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Regulation of Electron Density in Pt Nanoparticles via Bimetallic Metal-Organic Frameworks for Enhancing Photothermal Catalysis of Toluene Decomposition 通过双金属金属-有机框架调节铂纳米粒子中的电子密度,以增强甲苯分解的光热催化作用
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.2024.136561
Songyu Luo, Shipeng Fan, Jie Yuan, Jianyu Xiao, Xu Sun, Liang Wang, Yongfan Zhang, Zizhong Zhang, Xianzhi Fu, Wenxin Dai
Volatile Organic Compounds (VOCs) are omnipresent in the sphere of human industrial, harboring latent adverse consequences for health and the ecological system. The photothermal catalytic oxidation of VOCs is an advanced integrated technology that harnesses the combined effects of light and heat energy to enhance the efficiency of VOCs degradation. Herein, a bimetallic Metal-Organic Framework (MOF) was synthesized with the incorporation of Ce into the UiO-66-NH2(Zr) (i.e., UNH(Zr)), UiO-66-NH2(Zr2Ce) (i.e., UNH(Z2C)), which was achieved with Ce atom substituting for a portion of Zr atom within the Zr-oxo clusters. Pt nanoparticles (NPs) are integrated with MOFs to form composites using the dual-solvent method. Ce-oxo fulfills a bifunctional role: it not only facilitates the enhancement of the ligand-to-metal charge transfer (LMCT), but also establishes interaction with Pt NPs. Ce-oxo mediates an enhancement of electron density on Pt NPs. This phenomenon enhances the adsorption and activation of oxygen, significantly boosting the photocatalytic performance for toluene degradation, as demonstrated by a reduction of 30℃ for complete mineralization of toluene as compared to that of Pt@UiO-66-NH2(Zr) (i.e., PUNH(Zr)). This study potentially offers new insights into the relationship between electron transfer effects in bimetallic MOF-based catalysts and their efficient catalytic performance for VOCs degradation.
挥发性有机化合物(VOCs)在人类工业领域无处不在,对健康和生态系统潜伏着不利影响。VOCs 的光热催化氧化是一种先进的集成技术,它利用光能和热能的共同作用来提高 VOCs 的降解效率。本文合成了一种双金属金属有机框架(MOF),在UiO-66-NH2(Zr)(即UNH(Zr))、UiO-66-NH2(Zr2Ce)(即UNH(Z2C))中加入了Ce,实现了用Ce原子取代Zr-oxo团簇中的部分Zr原子。采用双溶剂法将铂纳米粒子(NPs)与 MOFs 结合形成复合材料。Ce-oxo 具有双重功能:它不仅能促进配体与金属之间的电荷转移(LMCT),还能与铂纳米粒子建立相互作用。Ce-oxo 可提高铂氮氧化物上的电子密度。与 Pt@UiO-66-NH2(Zr)(即 PUNH(Zr))相比,甲苯完全矿化的温度降低了 30℃,这表明这一现象增强了氧的吸附和活化,从而显著提高了光催化降解甲苯的性能。这项研究有可能为双金属 MOF 基催化剂中的电子转移效应与其高效降解挥发性有机化合物的催化性能之间的关系提供新的见解。
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引用次数: 0
The characteristic and bio-accessibility evaluation of mercury species in various kinds of seafood collected from Fujian of China for mercury risk assessment 从中国福建采集的各种海产品中汞物种的特征和生物可及性评价,用于汞风险评估
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.2024.136549
Chaochen Sun, Miaomiao Yin, Ying Peng, Chen Lin, Yongning Wu, FengFu Fu, Yue Lin
Seafood consumption is the major source of total Hg (tHg) and methyl mercury (MeHg) for humans. Lack of broad-representative bio-accessibility of mercury species makes accurate assessment on health risk of seafood’s mercury impossible. Herein, the concentrations and in vitro bio-accessibilities of mercury species in 93 seafood samples with 71 different species were extensively investigated. Results indicated that all shellfish and fish samples, and most seaweed samples contained both Hg2+ and MeHg, while some seaweed samples contained only Hg2+. The concentrations of mercury species varied depending on the differences in species/individuals of seafood and sampling regions. MeHg in seafood can be partly de-methylated into Hg2+ during gastrointestinal digestion, which reduced the toxicity of mercury in seafood. The mean demethylation rate of MeHg varied as follows: seaweeds (⁓62.1%) > shellfishes/shrimps (⁓19.7%) > fishes (⁓9.2%). The mean bio-accessibility of Hg2+ and tHg varied as follows: seaweeds (⁓97.7% and ⁓90.1%) > shellfishes/shrimps (⁓65.1% and ⁓67.9%) ≈ fishes (⁓65.1% and ⁓66.7%), while that of MeHg varied as follows: fishes (⁓57.7%) > shellfishes/shrimps (50.8%) > seaweeds (⁓11.6%). The simulated calculation of target hazard quotient (THQ) revealed that the health risk of seafood’s mercury may be accurately assessed using tHg, not mercury species, even without considering bio-accessibility. This offers a simple but protective approach for assessing the health risk of seafood’s mercury. Results of this study provide the potential broad-representative bio-accessibilities of mercury species existing in various kinds of seafood and novel insights for scientifically assessing the health risk of seafood’s mercury and revising the mercury limitation in seafood.
海产品是人类摄入总汞(tHg)和甲基汞(MeHg)的主要来源。由于缺乏具有广泛代表性的汞物种的生物亲和性,因此无法准确评估海产品中汞的健康风险。本文广泛研究了 71 个不同种类的 93 个海产品样本中汞的浓度和体外生物可及性。结果表明,所有贝类和鱼类样本以及大多数海藻样本都同时含有 Hg2+ 和 MeHg,而部分海藻样本仅含有 Hg2+。汞的种类浓度因海产品的种类/个体和采样地区的不同而异。海产中的甲基汞可在肠胃消化过程中部分脱甲基成为 Hg2+,从而降低海产中汞的毒性。甲基汞的平均脱甲基率变化如下:海藻类(⁓62.1%);贝类/虾类(⁓19.7%);鱼类(⁓9.2%)。Hg2+ 和 tHg 的平均生物可及性变化如下:海藻(⁓97.7% 和 ⁓90.1%)>;贝类/虾类(⁓65.1% 和 ⁓67.9%)≈鱼类(⁓18.1% 和 ⁓19.7%)>;鱼类(⁓9.2%)>。9%)≈鱼类(⁓65.1% 和⁓66.7%),而甲基汞的变化情况如下:鱼类(⁓57.7%)>;贝类/虾类(50.8%)>;海藻类(⁓11.6%)。目标危害商数(THQ)的模拟计算表明,即使不考虑生物可及性,海产品汞的健康风险也可以通过tHg而不是汞的种类来准确评估。这为评估海产品中汞的健康风险提供了一种简单但具有保护作用的方法。这项研究的结果提供了存在于各种海产品中的汞物种的潜在广泛代表性生物可及性,并为科学评估海产品汞的健康风险和修订海产品中汞的限制提供了新的见解。
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引用次数: 0
Biofilm formation mechanisms of mixed antibiotic-resistant bacteria in water: bacterial interactions and horizontal transfer of antibiotic-resistant plasmids 水中混合抗生素细菌的生物膜形成机制:细菌相互作用和抗生素质粒的水平转移
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.2024.136554
Longji Xia, Jiaping Wang, Min Chen, Guiying Li, Wanjun Wang, Taicheng An
Over 95% of bacteria on water supply pipeline surfaces exist in biofilms, which are hotspots for antibiotic resistance gene (ARG) transmission. This study established mixed biofilm culture systems on a metal iron substrate using Escherichia coli: antibiotic-sensitive bacteria (ASB) and antibiotic-resistant bacteria (ARB). The growth rate and extracellular polymeric substances (EPS) content of mixed biofilm surpassed single-species biofilms due to synergistic interactions among different bacteria. However, the composition of mixed biofilms formed by ASB and ARB became unstable after 72 h, linked to reduced polysaccharide proportions in EPS and inter-bacterial competition. The bacterial composition and conjugative transfer frequency of ARGs in mixed biofilms indicate that biofilm formation significantly enhances horizontal transfer of ARGs. Notably, the conjugative transfer frequency of the mixed biofilm formed by two ARB increased 100-fold within five days. In contrast, the conjugative transfer frequency in the mixed biofilm formed by ASB and ARB was unstable; inter-bacterial competition led to plasmid loss associated with horizontal transfer of ARGs, ultimately resulting in biofilm shedding. Furthermore, genes associated with ARG transfer and biofilm growth up-regulated by 1.5 − 6 and 2 − 7 times, respectively, in mixed biofilm. These findings highlight a mutually reinforcing relationship between biofilm formation and horizontal ARG transmission, with significant environmental implications.
供水管道表面 95% 以上的细菌存在于生物膜中,而生物膜是抗生素耐药基因 (ARG) 传播的热点。本研究利用大肠杆菌在金属铁基质上建立了混合生物膜培养系统:抗生素敏感菌(ASB)和抗生素耐药菌(ARB)。由于不同细菌之间的协同作用,混合生物膜的生长速度和胞外聚合物质(EPS)含量超过了单种生物膜。然而,ASB 和 ARB 形成的混合生物膜的组成在 72 小时后变得不稳定,这与 EPS 中多糖比例降低和细菌间竞争有关。混合生物膜中 ARGs 的细菌组成和共轭转移频率表明,生物膜的形成大大增强了 ARGs 的水平转移。值得注意的是,由两种 ARB 形成的混合生物膜的共轭转移频率在五天内增加了 100 倍。相比之下,ASB 和 ARB 形成的混合生物膜的共轭转移频率并不稳定;细菌间的竞争导致与 ARGs 水平转移相关的质粒丢失,最终导致生物膜脱落。此外,在混合生物膜中,与 ARG 转移和生物膜生长相关的基因分别上调了 1.5 - 6 倍和 2 - 7 倍。这些发现凸显了生物膜形成与 ARG 水平传播之间相辅相成的关系,对环境具有重要影响。
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引用次数: 0
Discovery of multiple bee-hazardous pesticides in ornamental plants via the Bee-Plex multi-target microsphere screening method 通过 Bee-Plex 多靶标微球筛选法发现观赏植物中多种危害蜜蜂的农药
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.2024.136556
Rubing Zou, Ruud van Dam, Nathalie Smits, Erik Beij, Toine Bovee, Dirk C. de Graaf, Yirong Guo, Jeroen Peters
Exposure to pesticides is one of the main drivers of global bee decline. However, the occurrence of pesticides in bee-attracting crops remains underexposed due to the lack of efficient on-site screening approaches for multi-analyte monitoring. Utilizing color-encoded superparamagnetic microspheres, we constructed a portable 8-plex indirect competitive microsphere-based immunoassay for the simultaneous determination of multiple bee-hazardous residues (Bee-Plex). Through a single measurement within 40 min, Bee-Plex exhibited high sensitivities with IC50values of 0.04, 0.08, 0.14, 0.15, 0.78, 0.86, 7.72, and 8.79 ng/mL for imidacloprid, parathion, fipronil, emamectin, carbofuran, chlorpyrifos, fenpropathrin and carbaryl, respectively. Moreover, the implementation of multiple broad-specific antibodies enables a wide-range screening profile for 30 pesticides and pesticide metabolites, detecting 6 neonicotinoids, 6 N-methyl carbamates 6 organophosphates, 5 avermectins, 5 pyrethroids and 2 phenylpyrazoles. The combination of Bee-Plex screening (93% accuracy) and LC-MS/MS confirmatory analysis revealed contaminations of neonicotinoids (100%) and avermectins (70%) in roses, with occurrence frequencies of 79%, 79%, 21%, 21%, 7%, and 7% for imidacloprid, acetamiprid, clothianidin, thiacloprid, imidaclothiz, and nitenpyram, respectively. Above all, this study offers a powerful analytical tool for rapid screening of multiple bee-hazardous pesticides, offering new insights in the occurrence of multi-pesticide contamination in ornamental plants.
接触农药是导致全球蜜蜂数量下降的主要原因之一。然而,由于缺乏高效的多分析物监测现场筛查方法,蜜蜂引诱作物中农药的发生率仍未得到充分暴露。利用彩色编码超顺磁性微球,我们构建了一种基于微球的便携式 8 重间接竞争性免疫测定法(Bee-Plex),用于同时测定多种危害蜜蜂的残留物。通过 40 分钟内的单次测定,Bee-Plex 表现出很高的灵敏度,对吡虫啉、对硫磷、氟虫腈、乙霉威、呋喃丹、毒死蜱、苯丙炔菊酯和西维因的 IC50 值分别为 0.04、0.08、0.14、0.15、0.78、0.86、7.72 和 8.79 纳克/毫升。此外,通过使用多种广谱特异性抗体,可对 30 种农药和农药代谢物进行大范围筛选,检测出 6 种新烟碱类、6 种 N-甲基氨基甲酸酯类、6 种有机磷类、5 种阿维菌素类、5 种拟除虫菊酯类和 2 种苯基吡唑类。结合 Bee-Plex 筛选(准确率达 93%)和 LC-MS/MS 确认分析,发现玫瑰中含有新烟碱类(100%)和阿维菌素类(70%),其中吡虫啉、啶虫脒、噻虫嗪、吡虫啉和硝虫嗪的出现频率分别为 79%、79%、21%、21%、7% 和 7%。总之,这项研究为快速筛选多种对蜜蜂有害的农药提供了一个强大的分析工具,为观赏植物中多种农药污染的发生提供了新的见解。
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引用次数: 0
The heterogenous molecular characteristics of biomass-pyrogenic smoke dissolved organic matters (BPS-DOMs) binding with PAHs: novel insights from combined analysis of FT-ICR MS and fluorescence variation 生物质烟气溶解有机物(BPS-DOMs)与多环芳烃结合的异质分子特征:从 FT-ICR MS 和荧光变化的联合分析中获得新见解
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.2024.136547
Huiying Zhang, Zhigeng Wang, Qin Dai, Jinzhi Ni, Yue Cheng, Ran Wei, Weifeng Chen
Biomass-pyrogenic smoke dissolved organic matter (BPS-DOM) can co-deposit with polycyclic aromatic hydrocarbons (PAHs), thereby altering their environmental behavior and fate in surface environments. However, the heterogeneous molecular characteristics of BPS-DOM binding with PAHs remain unclear. This study systematically elucidates the binding characteristics of PAHs (phenanthrene and pyrene), with various molecular compositions in BPS-DOM, utilizing FT-ICR MS and fluorescence variation analysis. CHO compounds in BPS-DOM, characterized by high aromaticity and abundant C=O bonds, significantly enhance PAHs binding by promoting π-π electron donor-acceptor interactions. In contrast, CHON compounds with higher aliphaticity inhibit pyrene binding by competing for binding sites on BPS-DOM. Furthermore, the binding sequence of different fluorescent molecules follows the order of CHO→CHOS→CHON for phenanthrene and CHO→CHON→CHOS for pyrene. This was primarily due to the larger conjugated aromatic structures of CHO compounds, which provide stronger π-π interaction sites for PAHs binding. The difference in binding sequences between phenanthrene and pyrene is primarily attributed to phenanthrene's reliance on π-π electron donor-acceptor interactions induced by -S=O and -N=O, while pyrene binding depended on π-π interactions driven by larger conjugated aromatic structures. These results provide an important theoretical foundation for further understanding the molecular-level interactions between BPS-DOM and PAHs.
生物质气相烟雾溶解有机物(BPS-DOM)可与多环芳烃(PAHs)共同沉积,从而改变其在地表环境中的环境行为和归宿。然而,BPS-DOM 与多环芳烃结合的异质分子特征仍不清楚。本研究利用 FT-ICR MS 和荧光变化分析,系统地阐明了不同分子组成的 PAHs(菲和芘)与 BPS-DOM 的结合特性。BPS-DOM 中的 CHO 化合物具有高芳香度和丰富的 C=O 键,可通过促进 π-π 电子供体与受体之间的相互作用显著增强 PAHs 的结合力。相反,脂肪族含量较高的 CHON 化合物通过竞争 BPS-DOM 上的结合位点来抑制芘的结合。此外,不同荧光分子的结合顺序依次为 CHO→CHOS→CHON 与菲结合,CHO→CHON→CHOS 与芘结合。这主要是由于 CHO 化合物的共轭芳香结构较大,为多环芳烃的结合提供了更强的π-π相互作用位点。菲和芘在结合顺序上的差异主要归因于菲依赖于 -S=O 和 -N=O 诱导的 π-π 电子供体-受体相互作用,而芘的结合依赖于较大共轭芳香结构驱动的 π-π 相互作用。这些结果为进一步了解 BPS-DOM 与多环芳烃之间的分子级相互作用提供了重要的理论基础。
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引用次数: 0
Metagenomics and metaproteomics reveal the effects of sludge types and inoculation modes on N,N-dimethylformamide degradation pathways and the microbial community involved 元基因组学和元蛋白组学揭示污泥类型和接种模式对 N,N-二甲基甲酰胺降解途径和相关微生物群落的影响
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.2024.136548
Yunchuan Xian, Linlin Cao, Yuxiang Lu, Qiuhong Li, Chengyuan Su, Yuan He, Guangrong Zhou, Shenglong Chen, Shu Gao
This study demonstrated the effects of the sludge type and inoculation method on the N,N-dimethylformamide degradation pathway and associated microbial communities. The sludge type is critical for DMF metabolism, with acclimatized aerobic sludge having a significant advantage in terms of DMF metabolism performance, whereas acclimatized anaerobic sludge has a reduced DMF metabolism capacity. Metagenomic revealed increased abundances of Methanosarcina, Pelomona and Xanthobacter in the adapted anaerobic sludge, suggesting that anaerobic sludge can utilize the methyl products produced by DMF metabolism for growth. Adapted aerobic sludge had high Mycobacterium abundance, significantly boosting DMF hydrolysis. In addition, a large number of dmfA2 genes were found in aerobic sludge, more so in acclimatized sludge, indicating stronger DMF metabolism. Conversely, acclimatized anaerobic sludge showed lower abundance of dmd-tmd and mauA/B, qhpA genes, implying long-term DMF toxicity reduced anaerobic microbial activity. Metaproteomic analysis showed that Methanosarcina and Methanomethylovorans enzymes in anaerobic sludge metabolized dimethylamine and methylamine to methane, aiding DMF degradation. In the aerobic sludge, aminohydrolase proteins, which hydrolyze DMF, were significantly upregulated. These findings provide insights into DMF wastewater treatment.
这项研究证明了污泥类型和接种方法对 N,N-二甲基甲酰胺降解途径和相关微生物群落的影响。污泥类型对DMF代谢至关重要,适应性好氧污泥在DMF代谢性能方面具有显著优势,而适应性厌氧污泥则降低了DMF代谢能力。元基因组显示,适应性厌氧污泥中 Methanosarcina、Pelomona 和 Xanthobacter 的丰度增加,表明厌氧污泥可以利用 DMF 代谢产生的甲基产物进行生长。适应性好氧污泥中的分枝杆菌数量较多,大大促进了 DMF 的水解。此外,在好氧污泥中发现了大量 dmfA2 基因,在适应性污泥中发现的更多,这表明 DMF 代谢更强。相反,适应性厌氧污泥中的 dmd-tmd 和 mauA/B, qhpA 基因丰度较低,这意味着长期的 DMF 毒性降低了厌氧微生物的活性。元蛋白组分析表明,厌氧污泥中的 Methanosarcina 和 Methanomethylovorans 酶可将二甲胺和甲胺代谢为甲烷,从而帮助降解 DMF。在好氧污泥中,水解 DMF 的氨水解酶蛋白明显上调。这些发现为 DMF 废水处理提供了启示。
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引用次数: 0
Coexposure to ambient air pollution and temperature and its associations with birth outcomes in women undergoing assisted reproductive technology in Fujian, China: A retrospective cohort study 中国福建接受辅助生殖技术的妇女对环境空气污染和温度的共同暴露及其与生育结果的关系:一项回顾性队列研究
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.2024.136539
Dongdong Jiang, Xuefen Cai, Hua Fang, Yuehong Li, Ziqi Zhang, Haoting Chen, Zixin Zheng, Wenxiang Wang, Yan Sun

Background

The interactions between pollutants and temperature coexposure, the mixing effects and their potential mechanisms remain uncertain.

Methods

This retrospective cohort study included 11,766 women with infertility who received treatment at Fujian Hospital between 2015 and 2024. The daily mean concentrations of the six pollutants and the relative humidity and temperature data were acquired from the Fujian region. Data on genes were obtained from the Comparative Toxicogenomics Database.

Results

O3 (aOR=0.80, 95% CI=0.725--0.891) and temperature (aOR=0.936, 95% CI=0.916--0.957) were negatively correlated with live birth rates. Moreover, PM10 (aOR=1.135, 95% CI=1.028--1.252) and PM2.5 (aOR=1.146, 95% CI=1.03--1.274) were positively associated with preterm birth. Among the effects on live births, PM2.5, PM10, NO2, CO, and SO2 had significant synergistic effects with temperature; in addition, O3 had significant antagonistic effects with temperature. A notable trend toward declining live birth rates with elevated concentrations of mixed pollutants was observed. Different infertility patients have different sensitivities to coexposure. Gene enrichment and cell experiments are associated mainly with cellular life activities.

Conclusions

Individual effects, interactions, and mixed effects between temperature and air pollutants and birth outcomes persist when air pollutant levels are relatively low. AAP may trigger miscarriage through cytotoxic effects.
方法这项回顾性队列研究纳入了2015年至2024年间在福建医院接受治疗的11766名不孕症妇女。六种污染物的日平均浓度以及相对湿度和温度数据均来自福建地区。结果O3(aOR=0.80,95% CI=0.725--0.891)和温度(aOR=0.936,95% CI=0.916--0.957)与活产率呈负相关。此外,PM10(aOR=1.135,95% CI=1.028--1.252)和 PM2.5(aOR=1.146,95% CI=1.03--1.274)与早产呈正相关。在对活产的影响中,PM2.5、PM10、二氧化氮、一氧化碳和二氧化硫与温度有显著的协同效应;此外,臭氧与温度有显著的拮抗效应。随着混合污染物浓度的升高,活产率呈明显下降趋势。不同的不孕症患者对共暴露的敏感性不同。结论当空气污染物水平相对较低时,温度和空气污染物与出生结果之间仍然存在个体效应、相互作用和混合效应。空气污染物可能通过细胞毒性效应引发流产。
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引用次数: 0
Conventional and biodegradable microplastics affected arsenic mobility and methylation in paddy soils through distinct chemical-microbial pathways 常规微塑料和可生物降解微塑料通过不同的化学-微生物途径影响砷在稻田土壤中的迁移和甲基化
IF 12.2 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-17 DOI: 10.1016/j.jhazmat.2024.136533
Hai-Qian Li , Jin-Peng Lv , Yue-Hui Jia , Jie Liu , Qiong Liang , Jian Zhou , Ai-Zhen Yang , Teng Yan , Yu-Ping Yang , Gui-Lan Duan
The presence of microplastics (MPs) in paddy soil has become a growing concern, yet the influence of MPs on arsenic (As) dynamics in paddy soil remains largely unexplored. A 98-day microcosm experiment was conducted to investigate the impact of MPs on As behavior in As-contaminated paddy soil. The results revealed that conventional microplastics (CMPs) reduced As concentration in porewater by 25–38 %, but substantially increased the percentage of methylated As (% MeAs) in soil by 8–23 times under 5 % dosages after 98-day incubation. In contrast, at the end of incubation, biodegradable microplastics (BMPs) at 5 % dosages notably increased As concentration in porewater and % MeAs in soil by 2–9 times and 11–395 times, respectively. The combination of network analysis and Random-Forest analysis implied that CMPs might inhibit As mobility through enhancing microbial As(III) oxidation and promote As methylation by enriching arsM-carrying microbes. However, BMPs promoted As release mainly accompanying with microbial iron reduction, and enhanced As methylation through enriching fermenting bacteria (i.e., Clostridiaceae) and arsM-carrying organic matter degrading bacteria (i.e., Gemmatimonas and Nocardia). These findings might provide broaden insights into As cycling induced by MPs and contribute to the prevention of combined pollution from As and MPs in paddy soil.
稻田土壤中微塑料(MPs)的存在已日益受到关注,但 MPs 对稻田土壤中砷(As)动态的影响在很大程度上仍未得到探讨。为了研究微塑料对砷污染稻田土壤中砷行为的影响,我们进行了为期 98 天的微生态系统实验。结果表明,传统微塑料(CMPs)可将孔隙水中的砷浓度降低 25-38%,但在 5% 的剂量下,经过 98 天的培养,土壤中甲基化砷的百分比(MeAs 百分比)大幅增加了 8-23 倍。相反,在培养结束时,生物可降解微塑料(BMPs)在 5% 的剂量下孔隙水中的砷浓度和土壤中甲基化砷的百分比分别显著增加了 2-9 倍和 11-395 倍。网络分析和随机森林分析的结合表明,CMPs 可能通过增强微生物 As(III) 氧化作用来抑制砷的迁移,并通过富集携带 arsM 的微生物来促进砷的甲基化。然而,BMPs 则主要通过微生物的铁还原作用促进砷的释放,并通过富集发酵菌(即梭状芽孢杆菌)和携带砷化氨的有机物降解菌(即革马提莫纳菌和诺卡氏菌)促进砷的甲基化。这些发现可能会拓宽人们对 MPs 诱导的砷循环的认识,并有助于防止砷和 MPs 对稻田土壤的联合污染。
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引用次数: 0
Affecting factors and health risks of organophosphate esters in urban soil and surface dust in a typical river valley city based on local bivariate Moran's I and Monte-Carlo simulation 基于局部双变量莫兰 I 和蒙特卡洛模拟的典型河谷城市土壤和地表尘埃中有机磷酸酯的影响因素和健康风险
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-16 DOI: 10.1016/j.jhazmat.2024.136534
Qian Zhang, Lijun Wang
A total of 102 urban soil and surface dust samples were collected from Lanzhou of China to clarify the occurrences, sources, affecting factors, and health risks of 13 organophosphate esters (OPEs). The total concentration of 13 OPEs (Ʃ13OPEs) in urban soil and surface dust ranged from 80.1 to 749 and 244 to 4905 ng/g, dominated by chlorinated OPEs (39.9% and 65.1%). The Ʃ13OPEs in the two media was higher in the central and eastern of Lanzhou due to local topography and wind direction. OPEs in the two media originated from industrial, traffic and commercial activities (37%–53.4%), atmospheric depositions (24.3%–31.3%), and OPEs-containing material emissions (14.5%–31.7%). Transport station number, residential/commercial area distribution, and road length were positively correlated with Ʃ13OPEs in the two media, suggesting that traffic activities are the main factors influencing the distribution of OPEs. Probabilistic non-cancer (< 1) and cancer (< 1×10-6) risks of human exposed to OPEs were low, mainly attributed to OPEs-containing material emissions (47.5%–62.0%) in urban soil and industrial/traffic activities (57.8%–92.2%) in surface dust. Reducing the frequency of human exposed to the two media and controlling the release of OPEs from pollution sources may mitigate population exposure risks.
为了明确 13 种有机磷酸酯(OPEs)的存在、来源、影响因素和健康风险,研究人员在中国兰州采集了 102 份城市土壤和地表灰尘样品。城市土壤和地表尘埃中 13 种 OPEs 的总浓度(Ʃ13OPEs)分别为 80.1 至 749 和 244 至 4905 ng/g,其中以氯化 OPEs 为主(39.9% 和 65.1%)。受当地地形和风向的影响,兰州中部和东部地区两种介质中的Ʃ13OPEs含量较高。两种介质中的 OPEs 来源于工业、交通和商业活动(37%-53.4%)、大气沉降(24.3%-31.3%)和含 OPEs 物质的排放(14.5%-31.7%)。交通站点数量、住宅/商业区分布和道路长度与两种介质中的Ʃ13OPEs 呈正相关,表明交通活动是影响 OPEs 分布的主要因素。人类暴露于 OPEs 的概率非致癌风险(1)和致癌风险(1×10-6)均较低,主要归因于城市土壤中的含 OPEs 物质排放(47.5%-62.0%)和地表扬尘中的工业/交通活动(57.8%-92.2%)。减少人类接触这两种介质的频率,并控制污染源释放的 OPEs,可降低人口接触风险。
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引用次数: 0
Cotransport of fullerene nanoparticles and clay colloids in porous media: the relation between aggregation and transport 富勒烯纳米颗粒与粘土胶体在多孔介质中的共传输:聚集与传输之间的关系
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-16 DOI: 10.1016/j.jhazmat.2024.136535
Weiyong Zhan, Guansheng Liu, Enzhu Hu, Jiaquan Zhang, Lili Huo, Hua Zhong
In the study, cotransport of fullerene nanoparticles (nC60) and mobile clay colloids (illite (ILL), kaolinite (KL), montmorillonite (ML)) in aquifer porous media and its relation to the aggregative interaction between these two types of particles was investigated. Minimal interaction occurred between nC60 and ILL, resulting in unaffected transport. Strong heteroaggregation between ML and nC60 resulted in not only significant retention of both particles during their cotransport but also the retention of nC60 in the media pre-injected with ML. Strong homoaggregation of KL caused strong straining effect and consequently retention of both KL and nC60 during their cotransport, however, did not cause retention of nC60 during the sequential injection of KL and nC60. Such aggregation behaviors were well demonstrated by the adsorption-sedimentation experiment, microscopic observation, the size and zeta-potential test, and model simulation. Based on the surface chemistry analysis, divalent-cation bridging between ML and nC60 and hydrogen bonding between KL particles were responsible for the heteroaggregation and the homoaggregation, respectively. The study demonstrated the specificity of the aggregation between the mobile clays and nC60 to the chemistry of the clays and its consequent effect on the cotransport of the particles, which is critical for assessment of the environmental risk of nC60.
本研究探讨了富勒烯纳米颗粒(nC60)和流动粘土胶体(伊利石(ILL)、高岭石(KL)和蒙脱石(ML))在含水层多孔介质中的共迁移及其与这两种颗粒之间聚集相互作用的关系。nC60 与 ILL 之间的相互作用极小,因此迁移不受影响。ML 和 nC60 之间的强烈异聚集不仅导致这两种粒子在共传输过程中大量保留,而且还导致 nC60 保留在预先注入 ML 的介质中。KL 的强烈同聚集会产生强烈的应变效应,从而在共传输过程中保留 KL 和 nC60,但在连续注入 KL 和 nC60 的过程中不会保留 nC60。吸附沉积实验、显微镜观察、粒度和 zeta 电位测试以及模型模拟都很好地证明了这种聚集行为。根据表面化学分析,ML 与 nC60 之间的二价阳离子桥和 KL 颗粒之间的氢键分别是异聚集和同聚集的原因。该研究证明了移动粘土和 nC60 之间的聚集与粘土化学的特异性及其对颗粒共迁移的影响,这对于评估 nC60 的环境风险至关重要。
{"title":"Cotransport of fullerene nanoparticles and clay colloids in porous media: the relation between aggregation and transport","authors":"Weiyong Zhan, Guansheng Liu, Enzhu Hu, Jiaquan Zhang, Lili Huo, Hua Zhong","doi":"10.1016/j.jhazmat.2024.136535","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136535","url":null,"abstract":"In the study, cotransport of fullerene nanoparticles (<em>n</em>C<sub>60</sub>) and mobile clay colloids (illite (ILL), kaolinite (KL), montmorillonite (ML)) in aquifer porous media and its relation to the aggregative interaction between these two types of particles was investigated. Minimal interaction occurred between <em>n</em>C<sub>60</sub> and ILL, resulting in unaffected transport. Strong heteroaggregation between ML and <em>n</em>C<sub>60</sub> resulted in not only significant retention of both particles during their cotransport but also the retention of <em>n</em>C<sub>60</sub> in the media pre-injected with ML. Strong homoaggregation of KL caused strong straining effect and consequently retention of both KL and <em>n</em>C<sub>60</sub> during their cotransport, however, did not cause retention of <em>n</em>C<sub>60</sub> during the sequential injection of KL and <em>n</em>C<sub>60</sub>. Such aggregation behaviors were well demonstrated by the adsorption-sedimentation experiment, microscopic observation, the size and zeta-potential test, and model simulation. Based on the surface chemistry analysis, divalent-cation bridging between ML and <em>n</em>C<sub>60</sub> and hydrogen bonding between KL particles were responsible for the heteroaggregation and the homoaggregation, respectively. The study demonstrated the specificity of the aggregation between the mobile clays and <em>n</em>C<sub>60</sub> to the chemistry of the clays and its consequent effect on the cotransport of the particles, which is critical for assessment of the environmental risk of <em>n</em>C<sub>60</sub>.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"166 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642825","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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