Emerging pollutants

新兴污染物
  • 文章类型: Journal Article
    导致产生活性氧(ROS)的氧活化对于光催化环境修复至关重要。当使用C3N4降解新出现的污染物时,O2吸附和还原活化的有限效率显着限制了ROS的产生。用金属单原子掺杂可能导致不令人满意的效率,由于光生电子-空穴对的复合。这里,将Mn和S单原子引入到C3N4中,产生了优异的光催化性能。Mn/S-C3N4可100%去除双酚A,速率常数是原始C3N4的11倍。根据实验结果和理论模拟,S原子限制空穴,促进光生载体分离。单原子Mn充当O2吸附位点,增强了对O2的吸附和活化,从而产生了ROS。这项研究提出了一种开发高效光催化剂的新方法,该方法遵循一种新的机制来消除水中的有机污染物。
    Oxygen activation leading to the generation of reactive oxygen species (ROS) is essential for photocatalytic environmental remediation. The limited efficiency of O2 adsorption and reductive activation significantly limits the production of ROS when employing C3N4 for the degradation of emerging pollutants. Doping with metal single atoms may lead to unsatisfactory efficiency, due to the recombination of photogenerated electron-hole pairs. Here, Mn and S single atoms were introduced into C3N4, resulting in the excellent photocatalytic performances. Mn/S-C3N4 achieved 100% removal of bisphenol A, with a rate constant 11 times that of pristine C3N4. According to the experimental results and theoretical simulations, S-atoms restrict holes, facilitating the photo-generated carriers\' separation. Single-atom Mn acts as the O2 adsorption site, enhancing the adsorption and activation of O2, resulting the generation of ROS. This study presents a novel approach for developing highly effective photocatalysts that follows a new mechanism to eliminate organic pollutants from water.
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  • 文章类型: Journal Article
    生物方法不能在低温下有效去除废水中的药品(PPs)和抗生素抗性基因(ARGs),导致环境污染。因此,设计了厌氧-好氧耦合的上流式生物电化学反应器(AO-UBER),以改善低温(10±2°C)下PPs的去除。结果表明,双氯芬酸(DIC)和布洛芬(IBU)在有好氧阳极和厌氧阴极室的系统中的去除率分别为91.7%和94.7%,高于控制系统(12.2±1.5%,36.5±5.9%),和好氧区有利于DIC和IBU的去除;有好氧阴极和厌氧阳极室的系统中氟喹诺酮类抗生素(FQs)的去除量比控制系统中的(9.1-22.4%)高17.5-22.4%,厌氧区有利于FQs的去除。微生物群落结构和ARGs分析表明,不同的电营养微生物(黄杆菌,不动杆菌,和Delftia)具有耐寒降解能力的PPs在不同的电极组合中富集,好氧阴极室可以去除某些ARGs。这些结果表明,间歇电刺激模式下的AO-UBER是在低温下有效去除PPs和ARGs的替代方法。
    Biological methods do not effectively remove pharmaceutical products (PPs) and antibiotic resistance genes (ARGs) from wastewater at low temperatures, leading to environmental pollution. Therefore, anaerobic-aerobic-coupled upflow bioelectrochemical reactors (AO-UBERs) were designed to improve the removal of PPs at low temperatures (10 ± 2 °C). The result shows that diclofenac (DIC) and ibuprofen (IBU) removals in the system with aerobic anodic and anaerobic cathodic chambers were 91.7% and 94.7%, higher than that in the control system (12.2 ± 1.5%, 36.5 ± 5.9%), and aerobic zone favors DIC and IBU removal; fluoroquinolone antibiotics (FQs) removals in the system with aerobic cathodic and anaerobic anodic chambers were 17.5-22.4% higher than that in the control system (9.1-22.4%), and anaerobic zone favors FQs removal. Analysis of microbial community structure and ARGs showed that different electrotrophic microbes (Flavobacterium, Acinetobacter, and Delftia) with cold-resistant ability to degrade PPs were enriched in different electrode combinations, and the aerobic cathodic chambers could remove certain ARGs. These results showed that AO-UBERs under intermittent electrical stimulation mode are an alternative method for the effective removal of PPs and ARGs at low temperatures.
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  • 文章类型: Journal Article
    氮掺杂生物炭作为类Fenton催化剂已被广泛用于去除废水中的新兴污染物。然而,原位和非原位氮掺杂对生物炭类Fenton催化活性的影响尚不清楚。在这项研究中,通过原位(NBC)和非原位(BC-N)氮掺杂制备了氮掺杂生物炭,并比较了NBC和BC-N对活化过氧化氢(H2O2)的类Fenton催化活性,过氧二硫酸盐(PDS)和过氧单硫酸盐(PMS)。结果表明,NBC比BC-N具有更高的类Fenton催化活性,因为碳量子点(CQDs)的形成显着增加了对H2O2,PDS和PMS的吸附能力。NBC可以激活H2O2,PDS和PMS降解磺胺甲恶唑(SMX),但表现出不同的催化活性和降解机理。在NBC/H2O2和NBC/PDS系统中,CQDs在H2O2和PDS的活化中起着关键作用,表面结合的反应性物种是SMX降解的主要原因。在NBC/PMS系统中,NBC既充当电子介体又充当激活剂,PMS和SMX之间的直接电子转移以及表面结合的反应性物种有助于SMX降解。这项研究提供了深入了解NBC对H2O2,PDS和PMS的催化活性。
    Nitrogen-doped biochar as Fenton-like catalysts has been widely used to remove emerging pollutants in wastewater. However, the effect of in-situ and ex-situ nitrogen doping on the Fenton-like catalytic activity of biochar is unclear. In this study, the nitrogen-doped biochar was prepared by in-situ (NBC) and ex-situ (BC-N) nitrogen doping, and the Fenton-like catalytic activity of NBC and BC-N was compared for activating hydrogen peroxide (H2O2), peroxydisulfate (PDS) and peroxymonosulfate (PMS). The results showed that NBC had higher Fenton-like catalytic activity than BC-N, because the formation of carbon quantum dots (CQDs) significantly increased the adsorption capacity to H2O2, PDS and PMS. NBC could activate H2O2, PDS and PMS for degradation of sulfamethoxazole (SMX), but showed different catalytic activity and degradation mechanism. In the systems of NBC/H2O2 and NBC/PDS, CQDs played a key role in the activation of H2O2 and PDS, and surface-bound reactive species were mainly responsible for SMX degradation. In the system of NBC/PMS, NBC acted as both electron mediator and activator, direct electron transfer between PMS and SMX and surface-bound reactive species contributed to SMX degradation. This study provides an insight into the catalytic activity of NBC for H2O2, PDS and PMS.
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  • 文章类型: Journal Article
    几丁质是第二丰富的天然生物聚合物,由β-(1→4)壳聚糖连接的N-乙酰葡糖胺单元组成,是几丁质的N-脱乙酰化产物。壳聚糖和甲壳素的性质,如生物相容性,无毒性质,和生物降解性,使它们成为能源和环境应用的成功替代品。然而,它们的低机械性能,小表面积,降低的热性能,和更大的孔体积限制了吸附应用的潜力。多项研究表明,可以通过用碳基复合材料制造壳聚糖和甲壳质来防止这些缺陷。本文对壳聚糖/甲壳素碳基材料的制备进行了全面分析。此外,这篇综述探讨了功能化壳聚糖/甲壳素生物聚合物的流行技术以及甲壳素和壳聚糖以及壳聚糖/甲壳素碳基复合材料的应用,在各种环境领域(减轻各种水污染物和开发生物传感器)。此外,随后的再生和吸附剂的再利用也进行了讨论。最后,我们总结了与利用壳聚糖/甲壳素碳基复合材料作为吸附剂去除水污染物相关的困难和潜在机会的简要概述。
    Chitin is the second most abundant natural biopolymer, which is composed of N-acetyl glucosamine units linked by β-(1 → 4) Chitosan is an N-deacetylated product of chitin. Properties of chitosan and chitin, such as biocompatibility, non-toxic nature, and biodegradability, make them successful alternatives for energy and environmental applications. However, their low mechanical properties, small surface area, reduced thermal properties, and greater pore volume restrict the potential for adsorption applications. Multiple investigations have demonstrated that these flaws can be prevented by fabricating chitosan and chitin with carbon-based composites. This review presents a comprehensive analysis of the fabrication of chitosan/chitin carbon-based materials. Furthermore, this review examines the prevalent technologies of functionalizing chitosan/chitin biopolymers and applications of chitin and chitosan as well as chitosan/chitin carbon-based composites, in various environmental fields (mitigating diverse water contaminants and developing biosensors). Also, the subsequent regeneration and reuse of adsorbents were also discussed. Finally, we summarize a concise overview of the difficulties and potential opportunities associated with the utilization of chitosan/chitin carbon-based composites as adsorbents to remove water contaminants.
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  • 文章类型: Journal Article
    新兴污染物(EP)在全球水生环境中普遍存在。研究人员努力在将它们释放到环境中之前了解它们的发生和行为。在这项研究中,我们检查了五个污水处理厂(WWTP),收集50个废水样品和10个污泥样品。我们使用质量平衡方程探索了这些WWTP中邻苯二甲酸酯(PAEs)的来源和目的地。废水处理降低了PAEs的频率和浓度,并降低了短链PAEs的比例。我们证实了初级治疗后PAEs浓度的增加,并修改了质量平衡方程。计算表明,冬季比夏季弱的“混合”和冬季比夏季强的沉降导致冬季废水处理对PAEs的去除效率很高。生物降解的质量通量受生物降解效率和收集的特定类型PAEs强度的组合影响,没有季节性差异。污泥沉降的质量通量主要受季节影响,冬季高于夏季。这项研究增强了我们对手动处理设施中新兴污染物的了解,并为优化水专业人员的废水处理方法提供了见解。
    Emerging pollutants (EPs) are prevalent in aquatic environments globally. Researchers strive to understand their occurrence and behavior prior to their release into the environment. In this study, we examined five wastewater treatment plants (WWTPs), collected 50 wastewater samples and 10 sludge samples. We explored the sources and destinations of phthalic acid esters (PAEs) within these WWTPs using mass balance equations. Wastewater treatment diminished the frequency and concentration of PAEs, and decreased the fraction of short-chain PAEs. We confirmed the increased concentration of PAEs post-primary treatment and modified the mass balance equation. Calculations suggest that weaker \"the mix\" in winter than in summer and stronger sedimentation in winter than in summer resulted in high efficiency of PAEs removal by winter wastewater treatment. The mass flux of biodegradation was influenced by the combination of biodegradation efficiency and the strength of the particular type of PAEs collected, with no seasonal differences. Mass fluxes for sludge sedimentation were mainly influenced by season and were higher in winter than in summer. This study enhances our understanding of emerging pollutants in manual treatment facilities and offers insights for optimizing wastewater treatment methods for water professionals.
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  • 文章类型: Journal Article
    多种新出现的污染物的共存给生物体的生态生理功能带来了巨大的负担。联合毒性和潜在机制需要深入了解。这里,选择海洋蓝贻贝(MytilusgalloprovincialisL.)并暴露于2,2\',4,4'-四溴二苯醚(BDE-47)和全氟辛酸(PFOA)在环境相关浓度下单独和组合使用,以阐明应激反应和潜在毒理学机制的差异。积累的表征和比较,生物标志物,组织病理学,进行转录组学和代谢组学。共同暴露导致不同的积累模式,加剧了组织病理学改变,以及在氧化应激和生物标志物中的不同反应。此外,发现贻贝中鉴定的差异表达基因(DEG)和差异代谢产物(DEM)被注释为不同的代谢途径。相关性分析进一步表明,DEG和DEM与上述生物标志物显著相关。BDE-47和PFOA改变了与氨基酸代谢相关的基因和代谢产物,能量和嘌呤代谢,ABC运输商,和不同程度的谷胱甘肽代谢,随后诱导积累差异和联合毒性。此外,本工作强调了Nrf2-keap1解毒途径在galloprovincialis适应BDE-47和PFOA诱导的活性氧(ROS)胁迫中的关键作用。这项研究使人们能够更全面地了解多种新兴污染物污染的联合毒性机制。
    The coexistence of multiple emerging contaminants imposes a substantial burden on the ecophysiological functions in organisms. The combined toxicity and underlying mechanism requires in-depth understanding. Here, marine blue mussel (Mytilus galloprovincialis L.) was selected and exposed to 2,2\',4,4\'-tetrabromodiphenyl ether (BDE-47) and perfluorooctanoic acid (PFOA) individually and in combination at environmental related concentrations to elucidate differences in stress responses and potential toxicological mechanisms. Characterization and comparison of accumulation, biomarkers, histopathology, transcriptomics and metabolomics were performed. Co-exposure resulted in differential accumulation patterns, exacerbated histopathological alterations, and different responses in oxidative stress and biomarkers for xenobiotic transportation. Moreover, the identified differentially expressed genes (DEGs) and differential metabolites (DEMs) in mussels were found to be annotated to different metabolic pathways. Correlation analyses further indicated that DEGs and DEMs were significantly correlated with the above biomarkers. BDE-47 and PFOA altered the genes and metabolites related to amino acid metabolism, energy and purine metabolism, ABC transporters, and glutathione metabolism to varying degrees, subsequently inducing accumulation differences and combined toxicity. Furthermore, the present work highlighted the pivotal role of Nrf2-keap1 detoxification pathway in the acclimation of M. galloprovincialis to reactive oxygen species (ROS) stress induced by BDE-47 and PFOA. This study enabled more comprehensive understanding of combined toxic mechanism of multi emerging contaminants pollution.
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  • 文章类型: Journal Article
    每天都有大量有毒物质和有害化学物质释放到外部环境中,对陆地和水生动物造成严重的环境影响。迄今为止,研究正在不断进行,以确定有效修复这些有害污染物的最佳催化材料。通过将功能性聚合物与无机纳米结构结合制备的杂化纳米材料由于其源自其整个纳米复合结构的显着多功能性能而成为有前途的研究领域。聚合物-无机杂化物中现有纳米材料设计的多功能性,关于它们的结构,composition,和建筑,为催化在环境修复中的应用开辟了新的前景。这篇评论文章提供了有关催化聚合物纳米复合材料的全面细节,并重点介绍了它们如何在有毒污染物的修复中充当催化剂。此外,它提供了制造聚合物纳米复合材料的设计和合成方法的处理的详细说明,并进一步探讨了精确设计方法的概念。聚合物纳米复合材料用于处理污染物(电催化,生物催化,催化,和氧化还原降解)。详细说明了经常使用的三种催化技术。此外,对上述催化过程和污染物的方法进行了广泛讨论。最后一部分总结了研究中的挑战以及催化聚合物纳米复合材料用于环境修复的潜力。
    A massive amount of toxic substances and harmful chemicals are released every day into the outer environment, imposing serious environmental impacts on both land and aquatic animals. To date, research is constantly in progress to determine the best catalytic material for the effective remediation of these harmful pollutants. Hybrid nanomaterials prepared by combining functional polymers with inorganic nanostructures got attention as a promising area of research owing to their remarkable multifunctional properties deriving from their entire nanocomposite structure. The versatility of the existing nanomaterials\' design in polymer-inorganic hybrids, with respect to their structure, composition, and architecture, opens new prospects for catalytic applications in environmental remediation. This review article provides comprehensive detail on catalytic polymer nanocomposites and highlights how they might act as a catalyst in the remediation of toxic pollutants. Additionally, it provides a detailed clarification of the processing of design and synthetic ways for manufacturing polymer nanocomposites and explores further into the concepts of precise design methodologies. Polymer nanocomposites are used for treating pollutants (electrocatalytic, biocatalytic, catalytic, and redox degradation). The three catalytic techniques that are frequently used are thoroughly illustrated. Furthermore, significant improvements in the method through which the aforementioned catalytic process and pollutants are extensively discussed. The final section summarizes challenges in research and the potential of catalytic polymer nanocomposites for environmental remediation.
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  • 文章类型: Journal Article
    在这项研究中,使用电离辐射在氧化石墨烯(R-Co-GO)表面上原位形成高度分散的纳米氧化钴,这对于激活PMS降解磺胺甲恶唑(SMX)非常有效。当在前体中使用150μL六水合氯化钴溶液时,R-Co-GO具有最高的催化活性,SMX降解的伪一级动力学常数为0.07min-1,矿化效率高(63.1%),PMS利用率高。硫酸根和高价钴氧是SMX降解的主要原因。机理分析表明,钴活性位点在PMS活化中占主导地位,它负责硫酸根和高价钴氧的形成;而碳框架有助于单线态氧的形成。R-Co-GO-150在5次循环实验中具有良好的催化活性和稳定性,其中SMX完全降解,溶解的Co浓度低于0.1mg/L此外,R-Co-GO-150/PMS体系也能降解苯酚,双酚A,阿特拉津和硝基苯有效,确认其广泛的适用性。这项研究提供了一种简单的方法,使金属氧化物均匀分散在碳材料表面,以及从实际废水中去除新出现的有机污染物的有效系统。
    In this study, ionizing radiation was used to induce the in-situ formation of highly dispersed nanosized cobalt oxide on the surface of graphene oxide (R-Co-GO), which was highly effective for activating PMS to degrade sulfamethoxazole (SMX). R-Co-GO had the highest catalytic activity when 150 μL cobalt chloride hexahydrate solution was used in the precursor, and the pseudo first-order kinetic constant of SMX degradation was 0.07 min-1 with high mineralization efficiency (63.1 %) and high PMS utilization efficiency. The sulfate radicals and high-valent cobalt oxo were mainly responsible for SMX degradation. Mechanism analysis showed that cobalt active site dominated in PMS activation, which was responsible for the formation of sulfate radicals and high-valent cobalt oxo; while the carbon framework contributed to the formation of singlet oxygen. The R-Co-GO-150 had good catalytic activity and stability in five cycling experiments, in which SMX was completely degraded and the concentration of dissolved Co was below 0.1 mg/L. In addition, the R-Co-GO-150/PMS system could also degrade phenol, bisphenol A, atrazine and nitrobenzene effectively, confirming its wide applicability. This study provided a facile method to uniformly disperse the metal oxides on the surface of carbon materials, and an effective system for the removal of emerging organic pollutants from the actual wastewater.
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  • 文章类型: Journal Article
    生物炭已成为一种多功能和高效的多功能材料,在从水生基质中去除新出现的污染物(EP)中既是吸附剂又是催化剂。然而,原始生物炭的催化和吸附能力受到其差的表面功能性和小孔径的阻碍。解决这些限制涉及功能化生物炭的开发,一种旨在增强其物理化学性质并提高吸附和催化效率的战略方法。尽管人们对这一领域的兴趣越来越大,现有文献存在显著差距,没有明确关注生物炭基功能材料(BCFMs)在水生环境中去除EP的功效的评论。这项全面的审查旨在通过深入研究设计具有增强的理化性质的BCFM所必需的工程考虑因素来填补这一空白。重点扩展到通过吸附或催化降解等机理来理解EP的处理效率。该综述系统地概述了BCFMs吸附和催化降解EPs的潜在机制。通过阐明BCFMs作为一种有前途的多功能材料的前景,审查强调了持续研究工作的必要性。它强调需要继续探索BCFMs的实际影响,特别是在与环境相关的污染物浓度下。这种整体方法旨在促进知识的发展,并应用基于生物炭的解决方案来应对水生生态系统中新兴污染物带来的挑战。
    Biochar has emerged as a versatile and efficient multi-functional material, serving as both an adsorbent and catalyst in removing emerging pollutants (EPs) from aquatic matrices. However, pristine biochar\'s catalytic and adsorption capabilities are hindered by its poor surface functionality and small pore size. Addressing these limitations involves the development of functionalized biochar, a strategic approach aimed at enhancing its physicochemical properties and improving adsorption and catalytic efficiencies. Despite a growing interest in this field, there is a notable gap in existing literature, with no review explicitly concentrating on the efficacy of biochar-based functional materials (BCFMs) for removing EPs in aquatic environments. This comprehensive review aims to fill this void by delving into the engineering considerations essential for designing BCFMs with enhanced physiochemical properties. The focus extends to understanding the treatment efficiency of EPs through mechanisms such as adsorption or catalytic degradation. The review systematically outlines the underlying mechanisms involved in the adsorption and catalytic degradation of EPs by BCFMs. By shedding light on the prospects of BCFMs as a promising multi-functional material, the review underscores the imperative for sustained research efforts. It emphasizes the need for continued exploration into the practical implications of BCFMs, especially under environmentally relevant pollutant concentrations. This holistic approach seeks to contribute to advancing knowledge and applying biochar-based solutions in addressing the challenges posed by emerging pollutants in aquatic ecosystems.
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  • 文章类型: Journal Article
    碳材料改性和缺陷工程对于增强卤化铋氧化物(BiOX)的光催化效率是必不可少的。在这项研究中,合成了一种新型多孔且富含缺陷的Ar-CB-2光催化剂,用于新兴污染物的降解。利用多壁碳纳米管(MWCNTs)的界面耦合效应,我们扩展了BiOI纳米片的吸收光谱,并显着抑制了电荷载流子的重组。通过氩气(Ar)等离子体蚀刻引入缺陷进一步增强了光催化剂的吸附效率和电子转移性能。与原始BiOI和CB-2相比,Ar-CB-2光催化剂表现出优异的光降解效率,随着四环素(TC)和双酚A(BPA)光降解的一级反应速率分别提高2.83和4.53倍,分别。进一步的探测实验表明,与CB-2/光系统相比,Ar-CB-2/光系统中·O2-和1O2的稳态浓度分别提高了1.67和1.28倍。该结果证实了Ar-CB-2的多孔和富含缺陷的结构抑制了电子-空穴复合并增强了光催化剂-氧相互作用,迅速将O2转化为活性氧,从而加速他们的生产。此外,预测了四环素和双酚A在Ar-CB-2/光体系中可能的降解途径。总的来说,这些发现为开发高效光催化剂提供了开创性的方法,能够迅速分解新出现的污染物。
    Carbon material modification and defect engineering are indispensable for bolstering the photocatalytic effectiveness of bismuth halide oxide (BiOX). In this study, a novel porous and defect-rich Ar-CB-2 photocatalyst was synthesized for emerging pollutants degradation. Leveraging the interfacial coupling effect of multi-walled carbon nanotubes (MWCNTs), we expanded the absorption spectrum of BiOI nanosheets and significantly suppressed the recombination of charge carriers. Introducing defects via Argon (Ar) plasma-etching further bolstered the adsorption efficacy and electron transfer properties of photocatalyst. In comparison to the pristine BiOI and CB-2, the Ar-CB-2 photocatalyst demonstrated superior photodegradation efficiency, with the first-order reaction rates for the photodegradation of tetracycline (TC) and bisphenol A (BPA) increasing by 2.83 and 4.53 times, respectively. Further probe experiments revealed that the steady-state concentrations of ·O2- and 1O2 in the Ar-CB-2/light system were enhanced by a factor of 1.67 and 1.28 compared to CB-2/light system. This result confirmed that the porous and defect-rich structure of Ar-CB-2 inhibited electron-hole recombination and boosted photocatalyst-oxygen interaction, swiftly transforming O2 into active oxygen species, thus accelerating their production. Furthermore, the possible degradation pathways for TC and BPA in the Ar-CB-2/light system were predicted. Overall, these findings offered a groundbreaking approach to the development of highly effective photocatalysts, capable of swiftly breaking down emerging pollutants.
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