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Photodegradation of polychlorinated biphenyls (PCBs) on suspended particles from the Yellow River under sunlight irradiation: QSAR model and mechanism analysis

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WATER RESEARCH 2024年 267卷 122547页

作者： Xu, Jianqiao Wei, Junyan Wei, Xinyuan Teng, Xiaolei Wang, Zunyao Qu, Ruijuan Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Jiangsu Peoples R China

Polychlorinated biphenyls (PCBs), as a class of hydrophobic organic pollutants, are widely found in river sediments and suspended particles, and the environmental fate of different PCBs can be better understood by investigating their photochemical transformation process. In this study, the quantitative structure-activity relationship (QSAR) model between the photodegradation rate constants of 17 PCBs adsorbed on Yellow River suspended particles in water (as a typical heterogeneous photodegradation system) and the physicochemical parameters of PCBs was constructed by SPSS and machine learning. The model showed that the more hydrophobicity of the molecule, the more positive charge carried by the aromatic C atoms, and the presence of chlorine atoms adjacent to the carbon bridge could all enhance the photochemical activity of PCBs. From the combined analysis of rate constants, quenching experiments and theoretical calculations, it was revealed for the first time that in natural suspended particle containing organic matter, the higher concentration of center dot O-2- and O-1(2) in the hydrophobic zone contributed more to the more hydrophobic PCBs, while center dot OH in the hydrophilic zone played a major role in the degradation of the less hydrophobic PCBs. Findings of this study would deepen the understanding of the degradation mechanism of hydrophobic pollutants by active species in complex environments.

关键词： Polychlorinated biphenyls Heterogeneous photodegradation QSAR model Machine learning Mechanism Active species

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Cross-Coupling of 1,2,3,4-Tetrachlororodibenzo-p-dioxin with Six Coexisting Polycyclic Aromatic Hydrocarbons during Photodegradation on a Fly Ash Surface

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ENVIRONMENTAL SCIENCE & TECHNOLOGY 2024年第46期58卷 20577-20587页

作者： Zhang, Ying Zhang, Shengnan Li, Xiaoyu Wang, Zunyao Qu, Ruijuan Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Jiangsu Peoples R China

The adverse conditions of the garbage incineration process can lead to the generation of dioxins and polycyclic aromatic hydrocarbons (PAHs). This study aimed to investigate the removal efficiency and possible cross-coupling effect of 1,2,3,4-tetrachlorodibenzo-p-dioxin (1,2,3,4-TCDD) and six coexisting low-molecular-weight PAHs during photodegradation on the fly ash surface. Due to their higher photoreactivity and light-shielding effect, the six PAHs exhibited inhibitory effects on the photodegradation of 1,2,3,4-TCDD, causing a reduction of 4.1%-21.2% in the removal efficiency. Common degradation products of 1,2,3,4-TCDD and PAHs were identified by LC-MS and GC-MS, and the formation of primary products was verified by theoretical calculations of bond dissociate energies, excitation energy, frontier electron densities, and transition states. In addition, high-molecular-weight coupling products of 1,2,3,4-TCDD and its interaction products with PAHs were observed in the mixed irradiation samples, and two coupling elimination mechanisms were proposed to illustrate their formation through C-O-C bonding and -COO- bonding, respectively. According to toxicity prediction analysis, the developmental toxicity and mutagenicity of most interaction products were higher than 1,2,3,4-TCDD. This study provided some new insights into the transformation, interaction, and related ecological risks of dioxins and PAHs coexisting on the surface of fly ash during the waste incineration process.

关键词： 1,2,3,4-tetrachlorodibenzo-p-dioxin polycyclic aromatichydrocarbons photochemical transformation interactionproducts theoretical calculation

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Potassium permanganate oxidation enhanced by infrared light and its application to natural water

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JOURNAL OF HAZARDOUS MATERIALS 2024年 464卷 133012页

作者： Guo, Ruixue Zhang, Shengnan Xiao, Xuejing Liang, Yeping Wang, Zunyao Qu, Ruijuan Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Jiangsu Peoples R China

Photocoupled permanganate (PM) is an effective way to enhance the oxidation efficiency of PM, however, the activation of PM by infrared has received little attention. This study aimed to investigate the ability of infrared light to activate PM. When coupled with infrared, the degradation rate of 4-chlorophenol (4-CP) is increased to 3.54 times of PM oxidation alone. The accelerated reaction was due to the formation of vibrationally excited PM by absorbing 3.1 kJ mol-1 infrared energy, which also leads to the primary reactive intermediates Mn(V/IV) in the reaction system. The infrared coupled PM system also showed 1.14-2.34 times promotion effect on other organic pollutants. Furthermore, solar composed of 45% infrared, coupled PM system showed excellent degradation performance, where the degradation of 4-CP in 10 L of tap water and river water was 68 and 23 times faster than in ultrapure water, respectively. The faster-increased degradation rate in natural waters is mainly due to the abundant inorganic ions, which can stabilize the manganese species, and then has a positive effect on 4-CP degradation. In summary, this work develops a energy-efficient photoactivated PM technology that utilizes infrared and provides new insights into the design of novel sunlight-powered oxidation processes for water treatment.

关键词： Potassium permanganate Infrared light Activation mechanism Natural water Practical application

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Insight into the photodegradation of o,p'-dichlorodiphenyltrichloroethane in a broad spectrum of irradiation light

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CHEMICAL ENGINEERING JOURNAL 2024年 488卷

作者： Cao, Wenqian Qi, Yumeng Zhang, Ying Guo, Ruixue Qu, Ruijuan Wang, Zunyao Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Jiangsu Peoples R China

Photolysis is the main pathway for the degradation of persistent organic pollutants (POPs). Most investigations, however, have been limited to the ultraviolet or visible region, and the reaction mechanism of infrared (IR) light is still unclear. In this study, the photodegradation of o,p '- dichlorodiphenyltrichloroethanes ( o,p '- DDT) on the silica (SiO 2 )/air interface under different irradiation light sources was systematically investigated. Interestingly, for the first time, effective degradation of o,p '- DDT under IR light irradiation was observed, which was ascribed to the anti -Stokes Raman scattering process of SiO 2 . Moreover, desert sands could also serve as a vector for the photodegradation of o,p '- DDT. The lower removal efficiency of desert sands compared to pure SiO 2 was a combined effect of differences in Fe 3+ component and SiO 2 content. It is worth noting that direct photodegradation plays a dominant role in the photodegradation of o,p '- DDT on SiO 2 . Besides, indirect photodegradation resulted mainly from center dot OH (25.0%), O 2 center dot - (6.9%), and 1 O 2 (5.6%) generated in the reaction system. In addition to hydroxylation and dechlorination products, the formation of four novel silicon -based products was observed, which resulted from the direct reaction of silyl radicals with o,p '- DDT. This study revealed that the specific Raman scattering effect of SiO 2 played a vital role in the self -purification process of POPs upon SiO 2 - based environmental matrices. The light -mediated decontamination system upon SiO 2 constructed in this study could provide critical information for addressing POPs contamination on sands.

关键词： o,p'-dichlorodiphenyltrichloroethane Silica/air interface Photodegradation Infrared (IR) light Silicon-based substitution products

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Effect of Dissolved Organic Matter on the Photodegradation of Decachlorobiphenyl (PCB-209) in Heterogeneous Systems: Experimental Analysis and Excited-state Theory Calculations

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ENVIRONMENTAL SCIENCE & TECHNOLOGY 2024年第32期58卷 14450-14459页

作者： Xu, Jianqiao Wei, Junyan Zhang, Jiayu Xing, Zhicheng Wang, Zunyao Qu, Ruijuan Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Jiangsu Peoples R China

Dissolved organic matter (DOM) can affect the transformation of pollutants through photosensitization, but most current research focuses on hydrophilic pollutants, making it such that less attention is paid to hydrophobic pollutants. In this paper, the effect and action mechanism of coexisting DOM on the photodegradation of decachlorobiphenyl (PCB-209) on suspended particles collected from the Yellow River were systematically investigated in a heterogeneous system using DOM standards and model compounds. Through molecular probe experiments, mass spectrometry analysis and theoretical calculations, we found that the excited triplet state of DOM ((DOM)-D-3*) could excite PCB-209 to undergo dechlorination reaction. Due to the different modes of electron transition, the presence of carbonyl groups decreased the energy of (DOM)-D-3*, whereas the electron-donating groups made the energy of (DOM)-D-3* higher. DOM containing phenolic hydroxyl groups led to a higher steady-state concentration of (OH)-O-center dot, and DOM containing phenyl ketone structures had a stronger ability to produce O-center dot(2)-. Compared with aqueous (OH)-O-center dot, O-center dot(2)- produced from hydrophobic microregions could react more readily with PCB-209. This study deepens the understanding of the role of different functional groups of DOM in the photosensitized transformation of hydrophobic compounds.

关键词： dissolved organic matter decachlorobiphenyl heterogeneous photodegradation functional groups active species

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Diversity and dynamic response of anaerobic ammonia oxidation granular sludge

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Journal of Environmental Sciences 2025年第6期152卷 262-275页

作者： Jiahong Ye Xiang Li Yan Yuan Yayi Wang Yong Huang JunMa Han Wang Pengze Dang Pei-ling Xu School of Environmental Science and Engineering Suzhou University of Science and TechnologySuzhou 215009China State Key Laboratory of Pollution Control and Resources Reuse Shanghai Institute of Pollution Control and Ecological SecurityCollege of Environmental Science and EngineeringTongji UniversityShanghai 200092China State Key Laboratory of Urban Water Resource and Environment Harbin Institute of TechnologyHarbin 150090China

Red anaerobic ammonia oxidation (Anammox) granular sludge (AnGS) has been reported insuccessfully operating Anammox systems, and its color is associated with sludge ***, in long-term operating systems, AnGS exhibits different sensory colors, physicalstructures, community structures, and denitrification performance, but the relationship betweenthem has not yet been *** AnGS of the Anammox system, which has beenin operation for more than a decade, can be divided into twomain categories: red and *** specific Anammox activity (SAA) in conventional red AnGS increased continuously asthe particle size increased from <0.51 mm to 6.02 ± 0.84 mm. The SAA of white AnGS wereslightly lower than those of red AnGS with similarly-size granules but significantly higherthan AnGS with smaller red granules. Compared with red AnGS, the extracellular polymericsubstances of white AnGS were significantly reduced,mainly due to the higher intracellulariron content, resulting in lower heme c concentration. Thus, heme c may prove not to bean evaluative tool for measuring Anammox activity. Red and white AnGS, whether throughself-aggregation or adsorption by hydroxyl apatite and other carriers, will face the fate ofinternal voids during particle size growth. White AnGS exhibited amore complex microbialcommunity than red AnGS. Candidatus Brocadia was abundant in red AnGS and the abundanceincreased with increasing granule size. Candidatus Kuenenia and Candidatus Jetteniamade significant contributions to denitrification in white AnGS. This study provides a newperspective on particle selection for anammox engineering applications.

关键词： Anaerobic ammonium oxidation granular sludge Sensory diversity Intracellular iron Heme Enzyme activity Microbial diversity

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PICRUSt2 functionally predicts organic compounds degradation and sulfate reduction pathways in an acidogenic bioreactor

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Frontiers of Environmental Science & Engineering 2022年第4期16卷 81-93页

作者： Jun Li Aimin Li Yan Li Minhui Cai Gan Luo Yaping Wu Yechao Tian Liqun Xing Quanxing Zhang State Key Laboratory of Pollution Control and Resources Reuse School of the EnvironmentNanjing UniversityNanjing 210023China Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological EngineeringNanjing University of Science and TechnologyNanjing 210094China

For comprehensive insights into the influences of sulfate on performance,microbial community and metabolic pathways in the acidification phase of a two-phase anaerobic system,a laboratory-scale acidogenic bioreactor was continuously operated to treat wastewater with elevated sulfate concentrations from 2000 to 14000 mg/*** results showed that the acidogenic bioreactor could achieve sulfate reduction efficiency of greater than 70%for influent sulfate content less than 12000 mg/*** sulfate induced the accumulation of volatile fatty acids(VPAs),especially propionate and butyrate,which was the primary negative effects to system performance under the high-sulfate ***-throughput sequencing coupled with PICRUSt2 uncovered that the accumulation of VFAs was triggered by the decreasing of genes encoding short-chain acyl-CoA dehydrogenase(EC:1.3.8.1),regulating the transformation of propanoyl-CoA to propenoyl-CoA and butanoyl-CoA to crotonyl-CoA of propionate and butyrate oxidation pathways,which made these two process hardly ***,genes encoding(EC:1.3.8.1)were mainly carried by order *** was the most abundant sulfate-reducing bacteria and identified as the primary host of dissimilatory sulfate reduction ftinctional *** analysis indicated the dissimilatory sulfate reduction process predominated under a low sulfate environment,but was not favored under the circumstance of *** the increase of sulfate,the assimilatory sulfate reduction process finally overwhelmed dissimilatory as the dominant sulfate reduction pathway in acidogenic bioreactor.

关键词： Acidogenic phase reactor High-sulfate wastewater Sulfate reduction Acidogenic fermentation PICRUSt2

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Acetylacetone effectively controlled the secondary metabolites of Microcystis aeruginosa under simulated sunlight irradiation

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Journal of Environmental Sciences 2024年第1期135卷 285-295页

作者： Xiaomeng Wang Yixin Luo Shujuan Zhang Lixiang Zhou Department of Environmental Engineering College of Resources and Environmental SciencesNanjing Agricultural UniversityNanjing 210095China The State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China

Inactivation of cyanobacterial cells and simultaneous control of secondary metabolites is of significant necessity for the treatment of cyanobacteria-laden ***(AcAc)has been reported a specific algicide to inactivate Microcystis aeruginosa(***)and an effective light activator to degrade *** study systematically investigated the photodegradation ability of AcAc under xenon(Xe)irradiation on the secondary metabolites of ***,mainly algal organic matter(AOM),especially toxic microcystin-LR(MC-LR).Results showed that AcAc outperformed H_(2)O_(2)in destructing the protein-like substances,humic acid-like matters,aromatic proteins and fulvic-like substances of *** MC-LR(250μg/L),0.05 mmol/L AcAc attained the same degradation efficiency(87.0%)as 0.1mmol/L H_(2)O_(2).The degradation mechanism of Xe/AcAc might involve photo-induced energy/electron transfer and formation of carbon center *** conditions(pH>9.0)were detrimental to the photoactivity of AcAc,corresponding to the observed degradation rate constant(k_(1)value)of MC-LR drastically decreasing to 0.0013 min^(-1)as solution pH exceeded *** PO_(4)^(3-)and HCO_(3)^(-)ions had obvious inhibition effects,whereas NO_(3)^(-)slightly improved k_(1)value from 0.0277 min^(-1)to 0.0321 min^(-1).The presence of AOM did not significantly inhibit MC-LR degradation in Xe/AcAc *** addition,the biological toxicity of MC-LR was greatly reduced after *** results demonstrated that AcAc was an alternative algicidal agent to effectively inactivate algal cells and simultaneously control the secondary metabolites after cell ***,the concentration and irradiation conditions should be further optimized in practical application.

关键词： Microcystis aeruginosa Photodegradation Acetylacetone Secondary metabolites Microcystin

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Toward a rapid and convenient nanoplastic quantification method in laboratory-scale study based on fluorescence intensity

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Frontiers of Environmental Science & Engineering 2024年第5期18卷 117-126页

作者： Ruiqi Yan Sen Lin Qian Ding Lei Zhang Xia Yu Wentao Zhao Qian Sui State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process School of Resources and Environmental EngineeringEast China University of Science and TechnologyShanghai200237China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China

The thorough investigation of nanoplastics(NPs)in aqueous environments requires efficient and expeditious quantitative analytical methods that are sensitive to environmentally relevant NP concentrations and convenient to *** analysis-based quantitative methods have been acknowledged as effective and rapid approaches for quantifying NP concentrations in laboratory-scale ***,we compared three commonly used optical response indicators,namely fluorescence intensity(FI),ultraviolet absorbance,and turbidity,to assess their performance in quantifying ***,orthogonal experiments were conducted to evaluate the influence of various water quality parameters on the preferred indicator-based quantification *** results revealed that FI exhibits the highest correlation coefficient(>0.99)with NP ***,the limit of quantification(LOQ)for various types of NPs is exceptionally low,ranging from 0.0089 to 0.0584 mg/L in ultrapure water,well below environmentally relevant *** variations in water quality parameters such as pH,salinity,suspended solids(SS),and humic acid,a robust relationship between detectable FI and NP concentration was ***,an increased matrix,especially SS in water samples,results in an enhanced LOQ for ***,the quantitative method remains applicable in real water bodies,especially in drinking water,with NP LOQ as low as 0.0157–0.0711 mg/*** exceeds the previously reported detectable concentration for 100 nm NPs at 40µg/mL using surface-enhanced Raman *** study confirms the potential of FI as a reliable indicator for the rapid quantification of NPs in aqueous environments,offering substantial advantages in terms of both convenience and cost-effectiveness.

关键词： Nanoplastic quantification Fluorescence intensity Drinking water Limit of quantification(LOQ) Matrix effects

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The profound review of Fenton process:What’s the next step?

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Journal of Environmental Sciences 2025年第1期147卷 114-130页

作者： Yimin Lin Junlian Qiao Yuankui Sun Hongyu Dong State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Department of Environmental Science School of Ecological and Environmental SciencesEast China Normal UniversityShanghai 200241China

Fenton and Fenton-like processes,which could produce highly reactive species to degrade organic contaminants,have been widely used in the field of wastewater ***,the chemistry of Fenton process including the nature of active oxidants,the complicated reactions involved,and the behind reason for its strongly pH-dependent performance,is the basis for the application of Fenton and Fenton-like processes in wastewater ***,the conflicting views still exist about the mechanism of the Fenton *** instance,reaching a unanimous consensus on the nature of active oxidants(hydroxyl radical or tetravalent iron)in this process remains *** review comprehensively examined the mechanism of the Fenton process including the debate on the nature of active oxidants,reactions involved in the Fenton process,and the behind reason for the pH-dependent degradation of contaminants in the Fenton ***,we summarized several strategies that promote the Fe(Ⅱ)/Fe(Ⅲ)cycle,reduce the competitive consumption of active oxidants by side reactions,and replace the Fenton reagent,thus improving the performance of the Fenton ***,advances for the future were proposed including the demand for the high-accuracy identification of active oxidants and taking advantages of the characteristic of target contaminants during the degradation of contaminants by the Fenton process.

关键词： Advanced oxidation process Fenton Hydroxyl radical Fe(IV) Wastewater treatment

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