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Acute, chronic, and behavioral toxicity of fluorine-free foams to earthworm species Eisenia fetida and Dendrobaena veneta 无氟泡沫对蚯蚓种类的急性、慢性和行为毒性研究
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143860
Roger Yeardley , Michael Penrose , Paola Rodríguez Montoyo , Mohamed Ateia
Aqueous film-forming foams (AFFF) containing per- and polyfluoroalkyl substances (PFAS) are widely used as fire suppressants. Due to rising health and environmental concerns, fluorine-free foams (F3) are being developed and tested as safer alternatives. However, the impact of these replacement products on ecologically important earthworms has not been adequately studied. This study addresses this gap by comparing the acute, chronic, and behavioral effects of two F3 formulations, BioEx Ecopol and Angus Fire Jetfoam, with a commonly used PFAS-containing AFFF, Buckeye, on two species of earthworms. Soil treated with BioEx Ecopol and Buckeye at the maximum 3% concentration did not cause significant acute mortality in Eisenia fetida, whereas Angus Fire Jetfoam resulted in 100% mortality at the same concentration. In a 28-day chronic test, weight loss was observed in Dendrobaena veneta worms exposed to soil treated with Angus Fire Jetfoam. Additionally, both Eisenia fetida and Dendrobaena veneta demonstrated almost complete avoidance of soils treated with any of the three foams at 3% concentration, indicating potential ecological effects despite lack of acute toxicity by two of the products. The differences in toxicity are likely due to the distinct chemical compositions and surfactant concentrations in these foams. BioEx Ecopol and Buckeye, despite their differing surfactant mixtures, exhibited lower acute toxicity, whereas Angus Fire Jetfoam's high mortality rate points to a potentially problematic chemical formulation. By understanding the toxicity of current formulations, this study supports the ongoing development and evaluation of new fire suppression products, supporting the creation of safer technologies.
含全氟烷基和多氟烷基物质(PFAS)的水成膜泡沫(AFFF)被广泛用作灭火剂。由于对健康和环境日益关注,无氟泡沫(F3)正在作为更安全的替代品进行开发和试验。然而,这些替代产品对生态上重要的蚯蚓的影响尚未得到充分的研究。本研究通过比较两种F3配方(BioEx Ecopol和Angus Fire Jetfoam)与常用的含有pfas的AFFF (Buckeye)对两种蚯蚓的急性、慢性和行为影响,解决了这一差距。在最大浓度为3%的土壤中,BioEx Ecopol和七叶树处理的土壤没有引起大飞天Eisenia fetida的显著急性死亡率,而在相同浓度下,Angus Fire Jetfoam的死亡率为100%。在一项为期28天的慢性试验中,观察到暴露于安格斯火焰喷射泡沫处理的土壤中的veneta石斛蠕虫体重减轻。此外,臭Eisenia fetida和Dendrobaena veneta几乎完全避免了三种浓度为3%的泡沫处理的土壤,这表明尽管两种产品缺乏急性毒性,但潜在的生态效应。毒性的差异很可能是由于这些泡沫中不同的化学成分和表面活性剂浓度。尽管BioEx Ecopol和Buckeye的表面活性剂混合物不同,但它们的急性毒性较低,而Angus Fire Jetfoam的高死亡率表明,这是一种潜在的有问题的化学配方。通过了解当前配方的毒性,本研究支持正在进行的新灭火产品的开发和评估,支持创建更安全的技术。
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引用次数: 0
New insights into typical biodegradable plastics in rapid pyrolysis: Kinetics, product evolution and transformation mechanism 典型生物降解塑料快速热解的新认识:动力学、产物演化和转化机理
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143834
Jiuli Ruan , Zheng Liu , Kang Gao , Lingling She , Jingyang Liu , Yuwen Guo , Feilong Zhang
Biodegradable plastics (BP) have undergone rapid development in the field of replacing traditional packaging plastics. However, their recycling and disposal systems are unclear, and the standards are different, causing new environmental pollution. The rapid and appropriate disposal of BP has become a worthy direction of exploration. Here, rapid pyrolysis technology was used to explore the recycling of BP, and the product evolution and transformation mechanism of typical BP (BP1∼BP4) were analyzed. The results show that the main reaction stages of BP pyrolysis are concentrated at approximately 260∼450 °C. Most of the heat treatment stages of BP conform to the random nucleation and nuclear growth model An (n = 1.5, 2, 2.5. 3). The gaseous products of BP pyrolysis were mainly 1, 3-butadiene. The top four pyrolysis components are the same for the liquid products of BP1, BP2, and BP4, which are mainly benzoic acid (42.54%–44.67%). However, the proportion of polycyclic aromatic substances in the products of the BP3 pyrolysis solution was as high as 63.85%. For the transformation mechanism, BP containing polylactic acid (PLA) and polybutylene terephthalate-adipate (PBAT) is mainly composed of C–O bond fractures at the ester group and intramolecular hydrogen transfer to form a carboxyl group and CC. This study of BP pyrolysis provides an important scientific basis and theoretical reference for its rational and rapid treatment and product recovery and reuse.
生物降解塑料(BP)在替代传统包装塑料领域得到了迅速发展。然而,它们的回收和处理制度不明确,标准不同,造成了新的环境污染。快速、合理处置BP已成为一个值得探索的方向。本文采用快速热解技术对BP的循环利用进行了探索,分析了典型BP (BP1 ~ BP4)的产物演化和转化机理。结果表明,BP热解的主要反应阶段集中在260 ~ 450℃左右。BP的大部分热处理阶段符合随机形核和核生长模型An (n = 1.5, 2,2.5)。3) BP热解的气态产物主要为1,3 -丁二烯。BP1、BP2、BP4液态产物热解组分前4位相同,主要为苯甲酸(42.54% ~ 44.67%)。而BP3热解产物中多环芳香族物质的比例高达63.85%。在转化机理上,含有聚乳酸(PLA)和聚对苯二甲酸丁二酯-己二酸酯(PBAT)的BP主要由酯基上的C-O键断裂和分子内氢转移形成羧基和CC组成,本研究为BP的合理快速处理和产品回收再利用提供了重要的科学依据和理论参考。
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引用次数: 0
Response of bacterial communities in desert grassland soil profiles to acid mine drainage pollution 荒漠草原土壤剖面细菌群落对酸性矿井水污染的响应
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143831
Jianfei Shi , Wenting Qian , Zhibin Zhou , Zhengzhong Jin
Acid mine drainage (AMD) causes serious environmental pollution, which imposes stresses on soil ecosystems. Therefore, it is critical to study the responses of soil bacterial communities to AMD pollution in ecologically fragile desert grasslands. Here, the bacterial community composition, structure, and assembly processes in vertical soil profiles of an AMD contaminated desert grassland were explored using 16S rRNA high-throughput sequencing. The results showed that the surface layers of the profiles exhibited lower pH and higher heavy metals (HMs) content due to AMD influence. The AMD contamination led to reduced bacterial diversity in the surface soil layer of the profiles and significantly changed the bacterial community composition and structure. Gradients in pH, TK, TN, and HMs were the main factors driving bacterial community variability. In contrast to the uncontaminated profile, deterministic processes were important in shaping soil bacterial community in the AMD contaminated profiles. These findings will enhance understanding about the responses of soil bacteria in desert grassland soil to the environmental changes caused by AMD contamination and will improve the remediation of AMD contaminated soil.
酸性矿井水造成了严重的环境污染,给土壤生态系统带来了压力。因此,研究生态脆弱荒漠草原土壤细菌群落对AMD污染的响应具有重要意义。本研究利用16S rRNA高通量测序技术,研究了AMD污染荒漠草地土壤垂直剖面中细菌群落组成、结构和组装过程。结果表明,由于AMD的影响,型材的表层pH值降低,重金属含量升高。AMD污染导致土壤表层细菌多样性降低,细菌群落组成和结构发生显著变化。pH、TK、TN和hm的梯度是驱动细菌群落变异的主要因素。与未污染剖面相比,确定性过程在AMD污染剖面的土壤细菌群落形成中起重要作用。这些研究结果将有助于了解荒漠草原土壤细菌对AMD污染环境变化的响应,并有助于AMD污染土壤的修复。
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引用次数: 0
Progress on the removal of PFAS contamination in water by different forms of iron-modified biochar 不同形式的铁改性生物炭去除水中PFAS污染的研究进展。
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143844
Binglu Teng , Zhenhua Zhao , Liling Xia , Jiangxuan Wu , Hailong Wang
Per- and polyfluoroalkyl substances (PFAS) contamination poses a significant threat to human health. Iron-modified biochar is an eco-friendly, cost-effective, and efficient adsorption material. There is a beneficial interaction between iron groups and biochar to remove PFAS from water through adsorption and degradation. The removal mechanism of the iron-modified biochar mainly includes advanced oxidation, iron group reduction, and adsorption. The adsorption mechanism shifted from being dominated by hydrophobic interactions to electrostatic interactions and ion exchange. Different forms of iron-modified biochar showed excellent removal of short-chain PFAS, which is not found in other modified biochar. Few existing studies have systematically investigated the role of various forms of iron-modified biochar in PFAS removal. Accordingly, this review explores the following areas, the synthesis methods of different forms of iron-modified biochar, the removal effect on long and short-chain PFAS, the key factors affecting removal capacity and the mechanisms of their interaction, the mechanism of PFAS removal, and the regeneration capacity of the composites. In this study, the potential of different forms of iron-modified biochar for PFAS remediation was explored in depth. To provide new ideas for subsequent studies of PFAS removal using iron-modified biochar.
全氟和多氟烷基物质(PFAS)污染对人类健康构成重大威胁。铁改性生物炭是一种环保、经济、高效的吸附材料。铁基团与生物炭之间存在有益的相互作用,通过吸附和降解去除水中的PFAS。铁改性生物炭的去除机理主要包括深度氧化、铁基还原和吸附。吸附机理由疏水相互作用为主转变为静电相互作用和离子交换为主。不同形式的铁改性生物炭对短链PFAS的去除效果较好,这是其他改性生物炭所没有的。现有的研究很少系统地研究各种形式的铁修饰生物炭在去除PFAS中的作用。为此,本文就不同形式铁修饰生物炭的合成方法、对长链和短链PFAS的去除效果、影响去除能力的关键因素及其相互作用机制、PFAS去除机理、复合材料的再生能力等方面进行了探讨。在本研究中,深入探讨了不同形式的铁修饰生物炭对PFAS的修复潜力。为后续铁改性生物炭去除PFAS的研究提供新的思路。
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引用次数: 0
Pollutants in urban runoff: Scientific evidence on toxicity and impacts on freshwater ecosystems 城市径流中的污染物:关于毒性和对淡水生态系统影响的科学证据。
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143806
Lorena Cojoc , Núria de Castro-Català , Ioar de Guzmán , Julene González , Maite Arroita , Neus Besolí-Mestres , Isabel Cadena , Anna Freixa , Oriol Gutiérrez , Aitor Larrañaga , Isabel Muñoz , Arturo Elosegi , Mira Petrovic , Sergi Sabater
Urban runoff effluents transport multiple pollutants collected from urban surfaces. which ultimately reach freshwater ecosystems. We here collect the existing scientific evidence on the urban runoff impacts on aquatic organisms and ecosystem functions, assessed the potential toxicity of the most common pollutants present in urban runoff, and characterized the ecotoxicological risk for freshwaters. We used the Toxic Units models to estimate the toxicity of individual chemicals to freshwater biota and observed that the highest ecotoxicological risk of urban runoff was associated to metals, polycyclic aromatic hydrocarbons (PAHs) and pesticides and, in a few cases, to phthalates. The potential risk was highest for copper and zinc, as well as for anthracene, fluoranthene, Di(2-ethylhexyl) phthlate (DEHP), imidacloprid, cadmium, mercury, and chromium. These pollutants had contrasting effects on freshwater biological groups, though the risk overall decreased from basal to upper trophic levels. Our analysis evidenced a lack of data on ecotoxicological effects of several pollutants present in urban runoff effluents, caused by lack of toxicity data and by the inadequate representation of biological groups in the ecotoxicological databases. Nevertheless, evidence indicates that urban runoff presents ecotoxicological risk for freshwater biota, which might increase if hydrological patterns become extreme, such as long dry periods and floods. Our study highlights the importance of considering both the acute and chronic toxicity of urban effluent pollutants, as well as recognizing the interplay with other environmental stressors, to design adequate environmental management strategies on urban freshwater ecosystems receiving urban runoff.
城市径流污水携带着从城市表面收集的多种污染物,最终到达淡水生态系统。在此,我们收集了有关城市径流对水生生物和生态系统功能影响的现有科学证据,评估了城市径流中最常见污染物的潜在毒性,并描述了其对淡水的生态毒理学风险。我们使用 "毒性单位"(Toxic Units)模型来估算各种化学品对淡水生物群的毒性,发现城市径流的最高生态毒理学风险与金属、多环芳烃(PAHs)和杀虫剂有关,在少数情况下还与邻苯二甲酸盐有关。潜在风险最高的是铜和锌,以及蒽、荧蒽、酞酸二(2-乙基己基)酯(DEHP)、吡虫啉、镉、汞和铬。这些污染物对淡水生物群体的影响截然不同,但总体风险从基底营养级到上层营养级依次降低。我们的分析表明,由于缺乏毒性数据以及生态毒理学数据库中生物组群的代表性不足,城市径流污水中存在的几种污染物的生态毒理学影响数据不足。不过,有证据表明,城市径流对淡水生物群构成生态毒理学风险,如果水文模式变得极端,如长期干旱和洪水,这种风险可能会增加。我们的研究强调了考虑城市污水污染物的急性和慢性毒性以及认识到与其他环境压力因素的相互作用的重要性,以便为接受城市径流的城市淡水生态系统设计适当的环境管理策略。
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引用次数: 0
Probing the potential mechanism of permethrin exposure on Alzheimer's disease through enantiomer-specific network toxicology, multi-spectroscopic, and docking approaches 通过对映体特异性网络毒理学、多光谱和对接方法,探索接触氯菊酯对阿尔茨海默病的潜在影响机制。
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143786
Tianzhu Guan , Ning Li , Ya Gao , Mingyuan Gao , Qin Hu , Yajun Gao , Lixia Xiao , Zhenquan Yang , Qiaoquan Liu
Latest observations indicated that exposure of organic environmental neurotoxins may increase the potential risk of Alzheimer's diseases (AD). As a suspected food-derived risk factor, permethrin, composed of cis-isomer and trans-isomer, is widely used as a broad-spectrum pyrethroid insecticide in agricultural crops for the arthropod pests controlling. Thus, evaluating the impact of permethrin exposure is of great importance to human health. In this study, we performed the toxicological network approach to decipher AD-related mechanisms of cis-permethrin and trans-permethrin. Based on the toxicological network construction and central network topological analysis, human serum albumin (HSA) was selected as the core targets in AD-related developing. From the analysis of the steady state and time-resolved fluorescence quenching of HSA in presence of permethrin mixture, it has been inferred that the nature of the quenching mainly originates from the dynamic modes. Experimentally, the thermodynamic parameters revealed hydrophobic interactions and van der Waals forces played a major role during quenching process. Tryptophan synchronous fluorescence spectra were blue shifted whereas the position of tyrosine synchronous spectra was red shifted during the complex formation. Three-dimensional fluorescence together with FT-IR experiment confirmed that permethrin caused the secondary structure changes in HSA. To better understand the binding patterns between HSA and cis/trans -permethrin, theoretical calculation and molecular docking were implemented. According to the electrostatic potential map, the electrophilic attack region corresponds for electron rich oxygen atoms, while the nucleophilic attack regions were mainly located at over the benzene rings and methyl on cyclopropane ring of permethrins. Docking results shown that cis-permethrin and trans-permethrin located in hydrophobic pocket nearby Domain IIA with the different binding affinity (−7.6 and −9.2 kcal/mol), which consistent with the competitive displacement experiment. All these findings generated in the present study facilitated the elucidation of the molecular mechanism details between permethrin mixture and HSA, which provided fresh insights into the links between environmental exposure and AD-related adverse health outcomes.
最新观察表明,接触有机环境神经毒素可能会增加阿尔茨海默病(AD)的潜在风险。氯菊酯由顺式异构体和反式异构体组成,是一种广谱拟除虫菊酯杀虫剂,广泛用于农作物的节肢动物害虫防治。因此,评估氯菊酯暴露对人体健康的影响非常重要。在本研究中,我们采用毒理学网络方法来解读顺式氯菊酯和反式氯菊酯的AD相关机制。在毒理学网络构建和中心网络拓扑分析的基础上,我们选择了人血清白蛋白(HSA)作为AD相关发育的核心靶标。通过分析HSA在菊酯混合物存在下的稳态和时间分辨荧光淬灭,推断出淬灭的性质主要来源于动态模式。实验结果表明,热力学参数显示疏水相互作用和范德华力在淬灭过程中发挥了主要作用。在复合物形成过程中,色氨酸同步荧光光谱发生蓝移,而酪氨酸同步光谱的位置发生红移。三维荧光和傅立叶变换红外光谱实验证实,菊酯导致了 HSA 二级结构的变化。为了更好地理解HSA与顺式/反式氯菊酯的结合模式,研究人员进行了理论计算和分子对接。根据静电位图,亲电攻击区域与富含电子的氧原子相对应,而亲核攻击区域主要位于氯菊酯的苯环和环丙烷环上的甲基。对接结果表明,顺式氯菊酯和反式氯菊酯位于领域 IIA 附近的疏水口袋中,其结合亲和力不同(-7.6 和 -9.2 kcal/mol),这与竞争置换实验结果一致。本研究的所有这些发现有助于阐明氯菊酯混合物与HSA之间的分子机理细节,为环境暴露与AD相关不良健康后果之间的联系提供了新的见解。
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引用次数: 0
Trace element uptake by macroalgae: Organic colloids as a source of metals, including Fe and rare earth elements 大型藻类对微量元素的吸收:作为金属来源的有机胶体,包括铁和稀土元素
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143849
Jean-Alix Barrat , Thierry Heulin , Germain Bayon , Matthieu Waeles , Laurent Chauvaud , Marie-Laure Rouget
We determined the concentrations of trace elements including Fe, Al, rare earth elements and Y (REY), in Ascophyllum nodosum, one of the most abundant brown macroalgae in the North Atlantic. Samples were collected in the Bay of Brest (Brittany, France) and in the estuary of its main contributing river. The Y/Ho, Al/Ga, and Zr/Hf ratios display values distinctive from seawater, but similar to the continental crust; an observation which we show cannot be explained by the incorporation of terrigenous particles, nor inorganic colloids. On the other hand, REY, Ga, Al, as well as other trace elements such as Th, Sc, Pb and Cr, correlate strongly with Fe abundances. Since all these elements are chiefly carried by organic colloids, we propose that colloidal uptake onto the surface of the algae controls the bioaccumulation of these metals. Their assimilation or internalization by algae requires biological pathways yet to be determined. This process is vital for these organisms, as organic colloids appear to be their main source of Fe, an essential nutrient. However, it also allows the accumulation of some potentially toxic metals in algae (e.g., Pb), with implications on the overall health of coastal ecosystems.
本文测定了北大西洋最丰富的褐藻之一——葡萄藻(Ascophyllum nodosum)中微量元素Fe、Al、稀土元素和Y (REY)的含量。样本采集于布列塔尼的布列斯特湾及其主要河流的入海口。Y/Ho、Al/Ga和Zr/Hf比值与海水值不同,与大陆地壳值相近;我们所观察到的现象不能用陆源粒子或无机胶体的结合来解释。另一方面,REY、Ga、Al以及其他微量元素如Th、Sc、Pb和Cr与Fe丰度密切相关。由于所有这些元素主要由有机胶体携带,我们认为胶体对藻类表面的吸收控制了这些金属的生物积累。它们被藻类同化或内化的生物学途径尚未确定。这个过程对这些生物至关重要,因为有机胶体似乎是它们的主要来源铁,一种必需的营养物质。然而,它也使一些潜在的有毒金属(例如铅)在藻类中积累,对沿海生态系统的整体健康产生影响。
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引用次数: 0
Valorization of waste pistachio shells to bimetallic magnetic hydrochar for sustainable dual-action wastewater remediation: A comprehensive study with mechanistic insights and life cycle assessment 废弃开心果壳转化为双金属磁性碳氢化合物的可持续双作用废水修复:一项具有机理见解和生命周期评估的综合研究
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143818
Monark Bhatt , Harshil Thakkar , Janki Patel , Miraj Patel , Sonal Thakore
This research outlines an integrated experimental and theoretical strategy for converting Pistachio-shells by hydrothermal carbonization into a bimetallic magnetic hydrochar (BMHC), for effective adsorptive-degradation of organic pollutants. Environmental sustainability of BMHC is supported by life cycle assessment(LCA). Adsorption experiments showed rapid and efficient dye (MB, CV) and antibiotic (TC) removal within 50 min, with >97% efficiency. The catalytic properties of BMHC, facilitated Peroxymonosulfate (PMS)-driven complete degradation of targeted contaminants, through ROS generation. DFT calculations demonstrated the regioselectivity for targeted moieties. The degradation intermediates were identified by LCMS and possible degradation pathways were derived. In-silico toxicity assessment of these intermediates confirmed the process safety. Employing 'Hook and Destroy' approach, BMHC demonstrated magnetic separation and reusability over five cycles. This extensive research demonstrates waste-to-resource conversion of Pistachio-shells to BMHC, with dual functionality in adsorption and degradation, as well as magnetic recoverability, which advocates its potency for water treatment solutions.
本研究概述了通过水热碳化将开心果壳转化为双金属磁性碳氢化合物(BMHC)以有效吸附降解有机污染物的综合实验和理论策略。生命周期评价(LCA)支持了BMHC的环境可持续性。吸附实验表明,在50 min内快速有效地去除染料(MB, CV)和抗生素(TC),效率达97%。BMHC的催化性能,促进了PMS驱动的目标污染物的完全降解,通过生成活性氧。DFT计算证明了目标部分的区域选择性。利用LCMS鉴定了降解中间体,并推导了可能的降解途径。这些中间体的硅毒性评估证实了该工艺的安全性。采用“Hook and Destroy”方法,BMHC在五个循环中演示了磁分离和可重用性。这项广泛的研究表明,开心果壳可将废物转化为资源,并具有吸附和降解的双重功能,以及磁可回收性,这表明其在水处理解决方案中的潜力。
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引用次数: 0
Cobalt doped g-C3N4 activated peroxymonosulfate for organic pollutant degradation: Alterations in cobalt species and reactive oxygen species 掺钴 g-C3N4 活化过硫酸盐降解有机污染物:钴物种和活性氧物种的变化。
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143763
Yuesen Wang , Yanchun Huang , Yi Chen , Luming Dou , Yi Ren , Naiwen Li , Bo Lai , Bo Tan
Cobalt-based materials are promising catalysts for activating peroxymonosulfate (PMS) to degrade organic pollutants. Among various cobalt-based catalysts, the alteration in cobalt species and the reactive species produced are not fully understood. Herein, four materials were synthesized by controlling synthesis methods and doping of g-C3N4 to regulate cobalt species. Through two methods, ZIF/Co and Co3O4, whose main cobalt species are Co–O/Co–N and CoO/O–CoO, were synthesized. On this basis, ZIF/Co–CN and Co3O4–CN were synthesized by adding g-C3N4. Then, the four materials were used to activate PMS for carbamazepine (CBZ) degradation, focusing on the correlation between active sites and reactive species. CoO/O–CoO mainly led to the formation of free radicals, while Co–N tended to produce non-free radicals. The addition of g-C3N4 would facilitate non-free radical catalysis by promoting the conversion of Co–O to Co–N and enhancing the catalytic role of C and N. Finally, the systems with a high proportion of non-free radicals showed better degradation performance when multiple pollutants co-existed, and reactive species may be selective to different pollutants. The findings have significance for the synthesis design of cobalt-based catalysts and the regulation of reactive species to degrade different pollutants practically.
钴基材料是一种很有前景的催化剂,可激活过一硫酸盐(PMS)降解有机污染物。在各种钴基催化剂中,钴物种的变化和产生的活性物种尚未完全清楚。本文通过控制合成方法和 g-C3N4 的掺杂来调节钴的种类,合成了四种材料。通过两种方法合成了 ZIF/Co 和 Co3O4,其主要钴物种为 Co-O/Co-N 和 Co=O/O-Co=O。在此基础上,加入 g-C3N4 合成了 ZIF/Co-CN 和 Co3O4-CN。然后,将这四种材料用于活化 PMS 以降解卡马西平(CBZ),重点研究了活性位点与反应物之间的相关性。Co=O/O-Co=O 主要导致自由基的形成,而 Co-N 则倾向于产生非自由基。最后,当多种污染物共存时,非自由基比例高的体系表现出更好的降解性能,而反应物种可能对不同污染物具有选择性。这些发现对钴基催化剂的合成设计和调节反应物种类以实际降解不同污染物具有重要意义。
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引用次数: 0
3D Pt@ZnAl-LDH catalyst on low-grade charcoal: A novel electrochemical platform for efficient textile dye degradation and glycerol oxidation 低级木炭上的 3D Pt@ZnAl-LDH 催化剂:高效纺织染料降解和甘油氧化的新型电化学平台。
IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-12-01 DOI: 10.1016/j.chemosphere.2024.143807
Mohammad Hossein Shahabifard , Sajjad Eftekhari , Kiana Parchami , Fatemeh Bahrami , Mohammad Askarian-Amiri , Azam Pirkarami , Nargess Yousefi-Limaee
The development of sustainable and efficient electrochemical processes is crucial for addressing global challenges related to water scarcity. In this study, we present a novel 3D core-shell electrocatalyst, Pt@ZnAl-LDH, supported on low-grade charcoal (LGC), which exhibits exceptional electrocatalytic activity for the degradation and decolorization of dye and the electrocatalytic conversion of glycerol to valuable C3 chemicals. The electrocatalytic degradation of methylene blue dye from water was investigated with a focus on the impact of temperature, pH, and dye concentration. The Pt@ZnAl-LDH/LGC anode demonstrates high selectivity for converting glucose into lactate and other C3 products, achieving an impressive 85% conversion rate at 0.5 V vs. Furthermore, the electrode achieves an exceptionally high level of selectivity for C3 products, reaching 86% at 2.2 V vs, significantly outperforming other electrodes. Theoretical calculations and electrochemical in situ techniques reveal that the incorporation of ZnAl-LDH enhances the adsorption of hydroxyl species, leading to improved glucose oxidation reaction performance. The 3D Pt@ZnAl-LDH/LGC catalyst optimizes glycerol adsorption, preventing the formation of unwanted intermediates and ensuring high activity and selectivity for C3 products. This work presents a novel electrocatalytic compound for the degradation of toxic dyes and the production of valuable C3 products using an inexpensive aqueous glucose oxidation method.
开发可持续的高效电化学工艺对于应对与水资源短缺有关的全球性挑战至关重要。在本研究中,我们提出了一种新型三维核壳电催化剂 Pt@ZnAl-LDH,该催化剂以低级木炭(LGC)为支撑,在染料降解和脱色以及甘油电催化转化为有价值的 C3 化学品方面表现出卓越的电催化活性。研究了水中亚甲基蓝染料的电催化降解,重点关注温度、pH 值和染料浓度的影响。Pt@ZnAl-LDH/LGC 阳极在将葡萄糖转化为乳酸和其他 C3 产物方面表现出很高的选择性,在 0.5 V vs 时达到了令人印象深刻的 85% 转化率。此外,该电极对 C3 产物的选择性也非常高,在 2.2 V vs 时达到了 86%,明显优于其他电极。理论计算和电化学原位技术表明,ZnAl-LDH 的加入增强了对羟基的吸附,从而改善了葡萄糖氧化反应的性能。三维 Pt@ZnAl-LDH/LGC 催化剂优化了甘油的吸附,防止了不需要的中间产物的形成,确保了 C3 产物的高活性和选择性。这项研究提出了一种新型电催化化合物,可利用廉价的水性葡萄糖氧化法降解有毒染料并生产有价值的 C3 产品。
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