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Mechanistic insight into the role of typical microplastics in chlorination disinfection: Precursors and adsorbents of both MP-DOM and DBPs

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JOURNAL OF HAZARDOUS MATERIALS 2024年 462卷 132716页

作者： Yan, Zhihao Qian, Hanyang Yao, Juanjuan Guo, Meng Zhao, Xiong Gao, Naiyun Zhang, Zhi Chongqing Univ Key Lab Three Gorges Reservoir Reg Ecoenvironm Minist Educ Chongqing 400045 Peoples R China Tongji Univ State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China

Microplastics (MPs) in drinking water are predominantly m. The leaching of MPs derived dissolved organic matters (MP-DOM) from 5 mu m polypropylene MPs (PP-MPs) and polystyrene MPs (PS-MPs) and the formation of MP-DOM... 详细信息

Microplastics (MPs) in drinking water are predominantly < 10 m. The leaching of MPs derived dissolved organic matters (MP-DOM) from 5 mu m polypropylene MPs (PP-MPs) and polystyrene MPs (PS-MPs) and the formation of MP-DOM derived disinfection byproducts during chlorination disinfection were first investigated. Comparably, PS-MPs are more vulnerable to chlorination and the primary attacks are on para C in aromatic side-chains via electrophilic Cl-substitution and oxidation by two-electron transfer. The O/C and Cl/C ratio of polystyrene MPs was linear and exponential versus initial available Cl-2 concentrations, respectively. The sig-nificant PS-DOM leaching was observed with initial available Cl-2 of 4.0 mg/L (USEPA recommended upper dose). As the initial available Cl(2 )concentration increased to 8.0 mg/L, the adsorption of chloro-phenolic-components of 200 Daltons in PS-DOM by 5 mu m PS-MPs was observed for the first time. Trichloromethane (TCM) was identified as the dominant disinfection byproduct with a formation potential of 60.3 +/- 7.8 and 73.7 +/- 9.8 mu g/mg for PS-DOM and PP-DOM, respectively. The derived TCM could adsorb onto PS-MPs followed the pseudo-second-order kinetic and Langmuir isotherm models. Extreme chlorination could reduce the maximal adsorption capacity of TCM on 5 mu m PS-MPs from 196.68 +/- 48.66 to 146.02 +/- 32.98 mu g/g. Thus, PS-MPs act as precursors and carriers of TCM in chlorination.

关键词： Microplastics Chlorination Leaching Dissolved organic matters Disinfection by-products and adsorption

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Stratified structure of membrane clogs observed in full scale cross-flow tubular ultrafiltration (UF) system: Fouling characterization and a proposed two-stage formation mechanism

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WATER RESEARCH 2024年 263卷 122133页

作者： Zhang, Yanyan Gong, Hui Liu, Qinpei Zhou, Shuyan Zhu, Danyang Dai, Xiaohu Tongji Univ Inst Carbon Neutral Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse 1239 Siping Rd Shanghai 200092 Peoples R China

Membrane fouling remains a significant challenge in wastewater treatment, hindering both efficiency and lifespan. This study reports a distinct phenomenon of stratified membrane clogging observed in a full-scale crossflow tubular ultrafiltration (UF) system treating sludge anaerobic digestion (AD) reject water. The distinct stratified structure, comprising inner and outer layers within the cake layer, has not been previously described. This research involved characterizing the filtration performance, analyzing membrane clog composition, and proposing a two-stage formation mechanism for the stratified clogs. It was revealed that higher inorganic and lower organic content in the outer layer compared to the inner layer. Acid and alkali treatments demonstrated the effectiveness of combined cleaning strategies. A mathematical model was developed to determine the critical conditions for stratified clog formation, influenced by membrane flux and cross-flow velocity (CFV). It is proposed that outer layer forms through long-term selective deposition, while the inner layer results from short-term dewatering within limited tubular space. High CFV (>2.5 m/s) prevents inner layer formation. Critical conditions for stratification occur at a flux of 18 L/m(2)/h with a CFV of 0.1 m/s or 65 L/m(2)/h with a CFV of 0.35 m/s. This study contributes a novel understanding of stratified membrane clogging, proposing a two-stage formation mechanism and identifying critical conditions, which provides insights for effective fouling control strategies and maintenance of operational efficiency for membrane systems.

关键词： Ultrafiltration (UF) membrane Crossflow velocity (CFV) Membrane bioreactor (MBR) Membrane fouling Anaerobic digestion (AD) reject water

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Insight into the effect of UVC-based advanced oxidation processes on the interaction of typical microplastics and their derived disinfection byproducts during disinfection

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JOURNAL OF HAZARDOUS MATERIALS 2024年 472卷 134597页

作者： Yao, Juanjuan Qian, Hanyang Yan, Zhihao Zhao, Xiong Gao, Naiyun Zhang, Zhi Chongqing Univ Key Lab Three Gorges Reservoir Reg Ecoenvironm Minist Educ Chongqing 40045 Peoples R China Tongji Univ State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China

The 10 mu m polystyrene and polyethylene-terephthalate microplastics (MPs), prevalent in finished drink water, were employed to investigate the effect of normal dosage UVC-based advanced-oxidation-processes (UVC-AOPs) on the interaction between MPs and their derived disinfection-byproducts (DBPs) during subsequent chlorination-disinfection, in the presence of Br-,- , for the first time. The results indicated that UVC/H2O2 caused higher leaching of microplastic-derived dissolved-organic-matter (MP-DOM), with smaller and narrower molecular-weight-distribution than UVC and UVC/peroxymonosulfate (UVC/PMS). The trihalomethanes (as dominant DBPs) molar-formation-potentials (THMs-MFPs) for MP-DOM leached in different UVC-AOPs followed the order of UVC/H2O2>UVC/PMS>UVC.>UVC/PMS>UVC. The adsorption of formed THMs, especially Br-THMs, back on MPs was observed in all MPs suspensions with or without UVC-AOPs pre-treatment. The Cl-THMs adsorption by MPs is more sensitive to UVC-AOPs than Br-THMs. The adsorption experiments showed that UVC-AOPs reduce the capacity but increase the rate of THMs adsorption by MPs, suggesting the halogen and hydrogen bonding forces governed the THMs adsorption rate while hydrophobic interaction determines their adsorption capacity. The UVC-AOPs pre-treatment sharply increased the total yield of THMs via both indirectly inducing MP-DOM leaching and directly increasing the THMs-MFPs of MPs by oxidation. 21.36-41.96% of formed THMs adsorbed back on the UVC-AOPs-pretreated MPs, which might increase the toxicity of MPs.

关键词： UVC-AOPs Microplastics MP-DOM DBPs Adsorption mechanism

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Optimization of the Determination of Methylmercury in Solid Matrix Samples

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BULLETIN OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY 2025年第1期114卷 1-9页

作者： Lei, Pei Zhang, Jin Kong, Yaqi He, Huan Zhong, Huan Nanjing Normal Univ Sch Environm Nanjing 210023 Peoples R China Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Peoples R China

Accurate quantification of neurotoxic methylmercury (MeHg) in environmental samples is crucial for exploring its formation, behaviors, and risks. Here, we developed and optimized an alkaline digestion-manual purge trap/gas chromatography-cold atomic fluorescence spectrometry (GC-CVAFS) method for the quantification of MeHg in solid matrix samples such as sediments, soils or sedimentary rocks. The alkaline digestion method yielded higher recoveries of MeHg than the acid extraction method. The manual purge trap/GC analysis enhanced the detection of MeHg by increasing the loading volume of the digestion solution, thereby facilitating the detection of lower concentrations of MeHg in the samples when compared to fully automated analysis. The optimized method achieved a method the limit of detection (LOD) of 0.0263 ngg-1 and a limit of quantification (LOQ) of 0.0876 ngg-1 with relative standard deviations of less than 10%. These results suggest that the alkaline digestion method is appropriate for the pretreatment and quantification of MeHg analysis in sediments or soils, particularly those from non-Hg contaminated sites.

关键词： Mercury Quantification Pretreatment Alkaline Digestion Acid Extraction

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A new process to further remove dissolved organic matter and disinfection by-product formation potential during drinking water treatment

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ENVIRONMENTAL SCIENCE AND pollution RESEARCH 2023年第8期30卷 20959-20969页

作者： Lei, Chongtian Chen, Yurong Li, Aimin Gao, Rui Zhang, Ziang Chen, Junxia Shi, Peng Zhou, Qing Ma, Yan Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse 163 Xianlin Ave Nanjing 210023 Jiangsu Peoples R China

Biological activated carbon (BAC) will produce soluble microbial products (SMPs), which affect effluent quality. To clarify the mechanism by which BAC affects effluent water quality, the processes of a drinking water plant in Jiangsu Province were investigated. It was found that during the O-3-BAC process, although ozonation could remove dissolved organic matter (DOC) to a certain extent, the DOC increased from 4.44 to 4.47 mg/L after BAC. Dissolved organic matter (DOM) in effluent from different processes was divided into five fractions based on hydrophilicity and hydrophobicity by resin fractionation. Through fluorescence excitation-emission matrix (EEM) spectroscopy combined with DOC analysis, it was found that SMPs are mainly included in transitional hydrophilic neutral (TPIN) fraction, which was the main cause of the DOC increase. Therefore, a new combined process was designed to remove TPIN effectively by coagulation after biological treatment, and found that coagulation had a good removal rate (13.2%) on TPIN. The trihalomethane formation potential (THMFP) of TPIN could be reduced effectively by 44.9% after coagulation. Compared with the old process, the new combined process had a higher removal rate (14.2-30.0%) of DOC, as well as a greater reduction of THMFP (29.0-78.6%) and haloacetic acid formation potential (HAAFP) (46.4-75.3%). This study aims to reveal the mechanism by which SMPs affect effluent water quality and exacerbate health risks, and to propose a solution to provide theoretical support for the design and optimization of drinking water treatment processes.

关键词： Dissolved organic matter (DOM) Biological activated carbon (BAC) Soluble microbial products (SMPs) Disinfection by-product formation potential (DBPFP) Coagulation

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Enhanced denitrification by graphene oxide-modified cathode for the secondary effluent of wastewater treatment plants in three-dimensional biofilm electrode reactors

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WATER SCIENCE AND TECHNOLOGY 2024年第12期89卷 3192-3207页

作者： Xue, Ying Zhang, Chaojie Li, Sibo Zhou, Qi Zhou, Xuefei Zhang, Yalei Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

In this study, a novel three-dimensional biofilm electrode reactor (3D-BER) with a graphene oxide (GO)-modified cathode was developed to enhance the denitrification performance of secondary effluent from wastewater treatment plants (SEWTPs). The effects of different HRTs and currents on the 3D-BER were explored. The results indicated that at the optimal HRT of 4 h and current of 350 mA/m(2), the 3D-BER with GO-modified cathode had a higher denitrification rate (2.40 +/- 0.1 mg TN/L/h) and less accumulation of intermediate products, especially with 3.34% TN molar conversion to N2O. The GO-modified cathode offered a large biocompatible specific surface area and enhanced the conductivity, which favored microbial growth and increased electron transfer efficiency and extracellular enzyme activities. Moreover, the activity of nitrite reductase increased more than that of nitrate reductase to accelerate nitrite reduction, thus facilitating the denitrification process. The proposed 3D-BER provided an effective solution to elevate tertiary denitrification in the SEWTP.

关键词： biofilm electrode reactors graphene oxide hydrogen autotrophic denitrification municipal wastewater

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Insights into enhanced oxidation of benzophenone-type UV filters (BPs) by ferrate(VI)/ferrihydrite: Increased conversion of Fe(VI) to Fe(V)/Fe(IV)

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SCIENCE OF THE TOTAL ENVIRONMENT 2024年 912卷 168860页

作者： Liu, Boying Zhang, Shengnan Liu, Mingzhu Cao, Siyu Qu, Ruijuan Wang, Zunyao Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Jiangsu Peoples R China Anhui Univ Sch Resources & Environm Engn Hefei 230601 Anhui Peoples R China

In this work, the oxidation performance of a new ferrate(VI)/ferrihydrite (Fe(VI)/Fh) system was systematically explored to degrade efficiently six kinds of benzophenone-type UV filters (BPs). Fe(VI)/Fh system not only had a superior degradation capacity towards different BPs, but also exhibited higher reactivity over a pH range of 6.0-9.0. The second-order kinetic model successfully described the process of BP-4 degradation by heterogeneous Fh catalyzed Fe(VI) system (R-2 = 0.93), and the presence of Fh could increase the BP-4 degradation rate by Fe(VI) by an order of magnitude (198 M-1 & sdot;s(-1) v.s. 14.2 M-1 & sdot;s(-1)). Remarkably, there are higher utilization efficiency and potential of Fe(VI) in Fe(VI)/Fh system than in Fe(VI) alone system. Moreover, characterization and recycling experiments demonstrated that Fh achieved certain long-term running performance, and the residual Fe content of solution after clarifying process meet World Health Organization (WHO) guidelines for drinking water. The contributions of reactive species could be ranked as Fe(V)/Fe(IV) > Fe(VI) > center dot OH. Fe(IV)/Fe(V) were the dominant species for the enhanced removal in the Fe(VI)/Fh system, whose percentage contribution (72 %-36 %) were much higher than those in Fe(VI) alone system (5 %-17 %). However, the contribution of Fe(VI) in oxidizing BP-4 should not be underestimated (20 %-56 %). These findings reasonably exploit available Fh resources to reduce the relatively high cost of Fe(VI), which offers a proper strategies for efficient utilization of high-valent iron species and may be used as a highly-efficient and cost-effective BPs purification method.

关键词： Benzophenone Ferrate Ferrihydrite Catalytic oxidation Fe(V)/Fe(IV) species

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Heterogenizing MnO2 nanostructure with industrial impurity ions for lead leakage-preventable anodes in zinc electrowinning

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JOURNAL OF HAZARDOUS MATERIALS 2024年 480卷 136259页

作者： Zhuang, Siwei Xu, Fuyuan Duan, Ning Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

gamma-MnO2 precoated lead (Pb)-based anodes have shown high initial activity in heavy-metal pollution reduction and production improvement for zinc electrowinning in laboratory. However, the accumulated impurity ions (M) in industrial MnO2-precursors restrict its industrial application. Herein, the heterostructure-induced rich oxygenvacancies for M-MnO2 and its higher activity (Pb/Co-MnO2>Pb/Ni-MnO2>Pb/Fe-MnO2 approximate to Pb/Cu-MnO2>Pb/MnO2) was reported. However, it reached a concentration threshold and afterwards provided the inhibited activity. Moreover, the Pb2+ diffusion-induced lead leakage is the dominant factor in the inactivation of anodes before extrinsic mechanical effects manifest, which follows: Pb/Fe-MnO2>Pb/Cu-MnO2 >Pb/MnO2 approximate to Pb/MnO2 approximate to Pb/Co-MnO2. Instead, due to the enhanced activity and suppressed lead leakage, Pb/Co-MnO(2 )avoided about 12.4 % and 72.3 % lead-containing anode slime in comparison with Pb/MnO2 and Pb/Fe-MnO(2 )and minimized the contamination of zinc products by lead. Such complex effects also provide a cost-effective and

关键词： Lead leakage MnO2 Impurity ions Heterostructure Zinc electrowinning

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Covalent organic framework in-situ immobilized laccase for the covalent polymerization removal of sulfamethoxazole in the presence of natural phenols: Prominent enzyme stability and activity

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JOURNAL OF HAZARDOUS MATERIALS 2024年 462卷 132714页

作者： Xu, Jiahui Zhang, Xiaomeng Zhou, Zhengwei Ye, Guojie Wu, Deli Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

In current water treatment processes, pollutants are typically degraded into small molecules and CO2 for detoxification. This study employed laccase-mediated aggregation of new pollutants with natural phenolic compounds to remove pollutants by forming large molecular substances, effectively sequestering carbon. Free laccase is susceptible to environmental influences, causing deactivation. However, immobilizing laccase onto a carrier enhances enzyme stability. In the experiment, laccase was immobilized onto the covalent organic framework TpPa-1 through an in-situ loading process, resulting in immobilized laccase Lac@TpPa-1. Stability studies revealed that immobilized laccase outperformed free laccase in terms of pH, temperature, and recyclability. Moreover, immobilized laccase was employed for catalyzing the removal of emerging pollutants containing natural phenolic compounds, achieving an 80.53% removal rate with the addition of 0.02 g of laccase within 5 h. Analytical techniques like Fourier-transform ion cyclotron resonance mass spectrometry were used to uncover reaction pathways, demonstrating the presence of radical polymerization and 1, 4 nucleophilic addition. This research utilized TpPa-1 as a carrier for laccase immobilization, promoting oxidation-induced polymerization for efficient pollutant removal. It provides a theoretical foundation for understanding the interplay between emerging pollutants and phenolic compounds in natural environments and enhances the practical application of laccase through immobilization.

关键词： Laccase Covalent organic framework Immobilization High activity and stability Oxidative polymerization process

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Synergistic strategy of solute environment and phase control of Pb-based anodes to solve the activity-stability trade-off

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JOURNAL OF HAZARDOUS MATERIALS 2024年 470卷 134119页

作者： Zhuang, Siwei Duan, Ning Xu, Fuyuan Tongji Univ Coll Environm Sci & Engn State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai 200092 Peoples R China

The contradiction between the activity and stability of metal anodes exists extensively, especially in acid electrooxidation under industrial -level current density. Although the anode modification enhanced the initial activity of anodes, its long-term activity is limited by anode slime accumulation. Herein, a synergistic strategy, coupling the solute environment with the phase control of anodes, is proposed to achieve the trade-off between activity and stability of Pb-based anodes in concentrated sulfuric acid electrolysis. Non -exogenous Mn2+ motivated a series of positive behaviours of reactive -oxygen -species capture, anode reconstruction and corrosion -dependent activity alleviation. The synergistic effects, which are crystal phase -dependent, mainly benefit from the continuous self -healing ability of the specific crystal phase of MnO2 on the anodes by the coexisted Mn2+. Compared with Mn2+/alpha-MnO2, Mn2+/gamma-MnO2 exhibited outperformed activity and stability in boosting oxygen evolution reaction (OER) and reducing hazardous pollutants, which resulted from the energy difference in the rate -determining step of OER and in the selectivity priority of Mn2+/MnO2 oxidation pathway. Interestingly, the pre -coated gamma-MnO2 on the anode also presents excellent inheritance, guaranteeing the unchanged crystal phase of MnO2 and the high performance in ultra -low hazardous slime generation in subsequent Mn2+ oxidation. The sustainability of Mn2+/gamma-MnO2 was proved in the operating hydrometallurgy conditions on Pb-based anodes. This strategy offers a promising approach for this common issue in electrooxidation-related areas.

关键词： Pb-based anodes Activity-stability trade-off Mn2+/MnO2 couple Reactive oxygen species Hydrometallurgy

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