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Considering the challenges for both single and traditional two-stage treatments, advanced oxidation and biodegradation, in the treatment of actual coking wastewater, an intimately coupled catalytic ozonation and biodegradation (ICOB) reactor was developed. In this study, ICOB treatment significantly enhanced the removal of Cu 2+ , Fe 3+ , and color by 39 %, 45 %, and 52 %, respectively, outperforming biodegradation. Catalytic ozonation effectively breaking down unsaturated organic substances and high-molecular-weight dissolved organic matter into smaller, more biodegradable molecules. Compared with biodegradation, the ICOB system significantly increased the abundances of Pseudomonas, Sphingopyxis, and Brevundimonas by ∼ 96 %, ∼67 %, and ∼ 85 %, respectively. These microorganisms, possessing genes for degrading phenol, aromatic compounds, polycyclic aromatics, and sulfur metabolism, further enhanced the mineralization of intermediates. Consequently, the ICOB system outperformed biodegradation and catalytic ozonation treatments, exhibiting chemical oxygen demand removal rate of ∼ 58 % and toxicity reduction of ∼ 47 %. Overall, the ICOB treatment showcases promise for practical engineering applications in coking wastewater treatment., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

The frequent occurrence of antibiotics in reclaimed water is concerning, in the case of managed aquifer recharge (MAR), it inevitably hinders further water purification and accelerates the evolutionary resistance in indigenous bacteria. In this study, we constructed two column reactors and nanoscale zero-valent iron (nZVI) amendment was applied for its effects on water quality variation, microbial community succession, and antibiotic resistance genes (ARGs) dissemination, deciphered the underlying mechanism of resistance risk reduction. Results showed that nZVI was oxidized to iron oxides in the sediment column, and total effluent iron concentration was within permissible limits. nZVI enhanced NO 3 - -N removal by 15.5% through enriching denitrifying bacteria and genes, whereas made no effects on oxacillin (OXA) removal. In addition, nZVI exhibited a pivotal impact on ARGs and plasmids decreasing. Network analysis elucidated that the diversity and richness of ARG host declined with nZVI amendment. Denitrifying bacteria play a key role in suppressing horizontal gene transfer (HGT). The underlying mechanisms of inhibited HGT included the downregulated SOS response, the inhibited Type-Ⅳ secretion system and the weakened driving force. This study afforded vital insights into ARG spread control, providing a reference for future applications of nZVI in MAR., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Due to the lack of normalized management, industrial waste is often co-disposed at open solid waste dumping sites, which could aggravate the groundwater pollution. In this study, 5 practical open solid waste dumping sites dealing with municipal solid wastes (MSW) (2 of 5) and industrial wastes mixed with MSW (3 of 5) were chosen to investigate the effect of waste co-disposal on the groundwater contamination. The industrial waste was mainly from rubber production, leather production, machinery industry, pharmaceutical industry and plastic production. 3 to 6 groundwater wells were excavated from each dumping site and 148 indices were analyzed, including regular chemicals, heavy metals, biological pollutants, volatile organic compounds (VOCs), semi-volatile organic compounds (SVOCs) and pesticide residues. Nemerow index analysis showed that 5 indices were severely polluted in the groundwater from every industrial waste co-disposal landfill, while only 0 and 1 severely polluted index was found for the two MSW landfill, respectively. The principal component analysis (PCA) analysis indicated that 2 biological pollutant (plate-counting bacteria (TPB) and total coliforms (TCs)), 4 chemical pollutants (permanganate index, ammonia, S 2- and petroleum) were closely connected with the disposal of industrial waste. Besides, co-disposal of industrial waste also brought in series of PAHs and dichloromethane, with di(2-ethylhexyl)phthalate exceeding the standard limit (10.5 mg L -1 ). Attention should be paid to TPB and TCs, whose maximal concentrations exceeded the standard limit by extraordinary 3200 and 1600 times, respectively. The distribution pattern of the pollutants showed that the biological pollutants at the downstream area, and chemical pollutants at the leakage points exhibited the highest concentration, which indicated the downstream area and seepage points should be specially concerned for the industry waste co-disposed dumping sites., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Due to its toxicity, the disinfection byproduct chlorite in drinking water is strictly regulated to be ≤ 1.0 mg/L, but in reclaimed, non-drinking water chlorite is unregulated and rarely considered. However, chlorite is cytotoxic and has a high oxidation potential. Therefore, as reclaimed water infiltrates soil and groundwater, it may alter the soil environment and microbial community, which may affect the degradation of organic matter and the transformation of the N element. In this study, the effects of reclaimed water containing chlorite on soil microorganisms were investigated by simulating subsurface infiltration. It was found that chlorite improved the conversion of nitrate nitrogen to nitrite nitrogen, but inhibited further conversion of nitrite nitrogen. The nitrite nitrogen in the effluent reached 4.61 mg/L when chlorite was present, while only 0.16 mg/L was found in the control system. The chlorite produced obvious oxidative stress reactions in cells, inhibited the EPSs production, in which the contents of polysaccharides and proteins reduced by nearly 41% and 62%, respectively. Besides, chlorite resulted in the enrichment of efflux resistance genes in the microbial community, mainly adeF and cmlB1. Self-protection against chlorite is achieved mainly using efflux pump related genes. Metagenomics data analysis showed that Delftia became the dominant genus when exposed to chlorite, with the greatest abundance at 17.9%. Chlorite also resulted in the upregulated expression of nar genes (by more than 149%) and downregulation of nir gene expression (by more than 62%). This study reveals the effects of the disinfection byproduct chlorite on a soil microecosystem, providing important information for the management and reuse of reclaimed water., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Coking wastewater contains high concentrations of cyanide, phenols, pyridine, quinoline, and polycyclic aromatic hydrocarbons. Its high toxicity and low biodegradability leads to long hydraulic retention time of biological process and high cost of advanced oxidation process. In this study, the simultaneous combination of ozonation and biodegradation (SCOB) was proposed to treat coking wastewater. Through this process, ozonation breaks the refractory organics, and the biodegradable intermediates are rapidly mineralized by microorganisms protected by porous carriers. Thus, the performances of SCOB, individual biodegradation and ozonation systems were compared. The long-term stability of the SCOB system was evaluated, the contributions of ozonation and biodegradation were analyzed, and their synergistic mechanisms were elaborated. Results showed that biological activity was inhibited in the biodegradation system, and chemical oxygen demand (COD) removal was only 27.6% for the ozonation system. COD and total phenol removal of SCOB system reached 48.5% and 79.3%, respectively, and its kinetic degradation constant of COD was 55.6% higher than that of the ozonation system. Ozonation contributed to the oxidation of organics with unsaturated functional groups as well as soluble microbial products (SMPs), causing the effluent toxicity and chroma to decrease by 82.7% and 270 times, respectively. The higher abundances of microorganisms and functions were enriched in the core of carrier, which became dominant region for biodegradation. Consequently, COD removal of the SCOB system stabilized at >80% for real coking wastewater treatment, confirming its promising potential for the treatment of highly polluted industrial wastewater., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Ammunition wastewater contains toxic nitrated explosives like RDX and oxyanions like nitrate and perchlorate. Its treatment is challenged by low efficiency due to contaminant recalcitrance and high cost due to multiple processes needed for separately removing different contaminant types. This paper reports a H 2 -based low-energy strategy featuring the treatment of explosives via catalytic denitration followed by microbial mineralization coupled with oxyanion reduction. After a nitrate- and perchlorate-reducing biofilm incapable of RDX biodegradation was coated with palladium nanoparticles (Pd 0 NPs), RDX was rapidly denitrated with a specific catalytic activity of 8.7 g cat -1 min -1 , while biological reductions of nitrate and perchlorate remained efficient. In the subsequent 30-day continuous test, >99% of RDX, nitrate, and perchlorate were coremoved, and their effluent concentrations were below their respective regulation levels. Detected intermediates and shallow metagenome analysis suggest that the intermediates after Pd-catalytic denitration of RDX ultimately were enzymatically utilized by the nitrate- and perchlorate-reducing bacteria as additional electron donor sources.

The quality of groundwater along rivers is greatly affected by long-term infiltration from surface water, especially reclaimed water-receiving rivers. To predict the degree of influence of contaminated river water on groundwater quality, the spatiotemporal distribution and migration evolution prediction of benzo[a]pyrene (B(a)P) was monitored and simulated by Hydrus-coupled Groundwater Modeling Systems (GMS) model in terms of reclaimed water-receiving Liangshui River. The prediction results indicated the goodness-of-fit of this coupled model, according to the model efficiency (E: 0.78-0.93), the mean absolute error (MAE: 0.01-0.32 m) and the root-mean-square error (RMSE: 0.06-0.35 m). The vertical infiltration rate of B(a)P in the vadose zone was 0.102 m -1 , which was only 0.73% that of water. B(a)P penetrated the 16 m depth vadose zone for 63 years owing to the attenuation function of adsorption and biodegradation, with contribution ratios of 78.4% and 19.3%, respectively. However, once B(a)P intersects with groundwater, the migration of B(a)P is dominated by horizontal migration due to downward movement along the groundwater flow direction. The migration rate of B(a)P in groundwater was 6.65 m/y in the horizontal direction, which was 2.42 and 16.22 times higher than the dispersion rate in the longitudinal and vertical directions, respectively. The spatiotemporal distribution indicated that the B(a)P concentration decreased with the crow-fly distance from river with attenuation rate constants of 1.19 × 10 -4 , 3.05 × 10 -4 , and 3.67 × 10 -3  m -1 over horizontal, longitudinal, and vertical direction, respectively, which were negatively correlated with migration rate. However, the B(a)P content increased over the extension of infiltration time with an accumulation rate of 7.3 × 10 -2 d -1 . The migration and accumulation of B(a)P induced potential health risks to groundwater-based drinking water safety, which resulted in the groundwater safety utilization range decreasing from 450 m, 283 m, and 20.1 m-583 m, 338 m, and 28.2 m far from the river over the horizontal, longitudinal, and vertical directions, respectively, 20 years later. This study provides a numerical modeling solution for the viable spatiotemporal evolution of B(a)P in groundwater and an effective decision-making tool for the safe utilization of groundwater as drinking water., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

In this study, a new intimately coupling technology of advanced oxidation and biodegradation was proposed, called simultaneous combination of ozonation and biodegradation (SCOB), which uses ozonation in place of traditional photocatalysis. SCOB was evaluated for its ability to degrade and detoxify tetracycline hydrochloride (TCH). Biodegradation alone only resulted in negligible TCH removal, while ozone alone caused less effective performance, with TCH degradation rate constants of 29-171% lower than those of SCOB. The optimal ozone dose was 2.0 mg-O 3 /(L·h), and it contributed to remove 97% of the TCH within 2 h under SCOB operation. The SCOB effluent was not toxic to S. aureus after 8 h of exposure. During six SCOB operation cycles, the biomass in the biofilm remained stable, and cell structure was relatively intact. SCOB significantly improved TCH degradation and reduced toxicity of the effluent., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Reducing energy use is crucial to commercialize electrochemical oxidation technologies. We developed a three-dimensional (3-D) electrochemical system that can significantly reduce the applied voltage and effectively degrade organic contaminants in low-ionic-strength wastewaters. The 3-D system consisted of a composite wire mesh anode (composed of blue TiO 2 nanotubes covered with SnO 2 -Sb 2 O 3 ), a proton exchange membrane, and a stainless-steel wire mesh cathode, which were compressed firmly together. For the 3-D system, we placed the anode of a 3-D electrode toward the wastewater that flowed past the anode. Both the two-dimensional (2-D) and 3-D systems had the same anode and cathode. We found that the 3-D system could reduce the applied voltage by 75.7% and reduce the electrical efficiency per log order reduction (EE/O) by 73% for 0.001 M Na 2 SO 4 . For Na 2 SO 4 concentrations greater than 0.05 M, the 2-D system had a slightly lower EE/O. We also compared the EE/O of electrochemical advanced oxidation processes (EAOPs) with that of other advanced oxidation processes (UV/H 2 O 2 , UV/persulfate, O 3 /H 2 O 2 , UV/ TiO 2 , and UV/chlorine). We found that EAOPs have a much higher EE/O for low BA concentrations (20 mg/L) and a much lower EE/O for high BA concentrations (2000 mg/L).

Intimately coupled photocatalysis and biodegradation (ICPB) is a promising technology for treating wastewater containing antibiotics. While past work has documented the benefits of ICPB for removing and mineralizing antibiotics, its impacts on mitigating biotoxicity from products has not been studied. We fabricated an ICPB carrier by coating Ag-doped TiO 2 on the outer skeleton of sponge carriers and allowing biofilm to grow in the internal macro-pores. We used amoxicillin (C 16 H 19 N 3 O 5 S) as the model antibiotic. The amoxicillin-removal rate contents with ICPB was greater by 40% vs. photocatalysis and 65% vs. biodegradation, based on the first-order kinetic simulation. While mineralization of amoxicillin was minimal for photocatalysis or biodegradation alone, it was ∼35% with ICPB. Photocatalysis alone led to accumulation of C 14 H 21 N 3 O 2 S; biodegradation alone resulted in accumulation of C 14 H 21 N 3 O 3 , C 16 H 18 N 2 O 4 S, and C 15 H 21 N 3 O 3 ; but they were negligible after ICPB. As a result, ICPB reduced toxicity impacts measured by Staphylococcus aureas growth, Daphnia magna mobility, and teratogenicity to Zebrafish embryos. In contrast, photocatalysis alone increased each of the toxicity effects. In sum, ICPB gave greater removal and mineralization of amoxicillin, and it mitigated biotoxicity from treatment products., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Recently, the UV/free chlorine process has gained attention as a promising technology for destroying refractory organic contaminants in the aqueous phase. We have developed a kinetic model based on first-principles to describe the kinetics and mechanisms of the oxidation of organic contaminants in the UV/free chlorine process. Substituted benzoic acid compounds (SBACs) were chosen as the target parent contaminants. We determined the second-order rate constants between SBACs and reactive chlorine species (RCS; including [Formula: see text], [Formula: see text] and [Formula: see text]) by fitting our model to the experimental results. We then predicted the concentration profiles of SBACs under various operational conditions. We analyzed the kinetic data and predicted concentration profiles of reactive radicals ([Formula: see text] and RCS), we found that [Formula: see text] was the dominant radicals for SBACs destruction. In addition, we established quantitative structure activity relationships (QSARs) that can help predict the second-order rate constants for SBACs destruction by each type of reactive radicals using SBACs Hammett constants. Our first-principles-based kinetic model has been verified using experimental data. Our model can facilitate a design for the most cost-effective application of the UV/free chlorine process. For example, our model can determine the optimum chlorine dosage and UV light intensity that result in the lowest energy consumption.

Anaerobic oxidation of methane (AOM) microorganisms widespread in nature and they are able to utilize methane as electron donor to reduce sulfate, nitrate, nitrite, and high valence metals. However, whether persistent organic contaminants can also be degraded remains unknown. In this study, the organic pollutant methyl orange (MO) was used to address this open question. The initial concentration of MO affected its degradation efficiency and higher concentration (>100 mg/L) caused considerable inhibition. A 13 CH 4 isotope experiment indicated that methane oxidation was involved in MO degradation, which produced N, N-dimethyl-p-phenylenediamine, and 4-aminobenzenesulfonic acid corresponded stoichiometrically. During the long-term experiment, the maximum degradation rate was 47.91 mg/(L·d). The percentage of Candidatus Methanoperedens and Pseudoxanthomonas significantly increased after 30-d of MO degradation under CH 4 conditions; moreover, Candidatus Methanoperedens dominated (46.83%) the microbial community. Candidatus Methanoperedens, either alone or in combination with Pseudoxanthomonas, utilized methane as the sole carbon source to degrade MO via direct interspecies electron transfer or the syntrophy pathway. This study will add to our understanding of the functions and applications of AOM microorganisms., (Copyright © 2018 Elsevier B.V. All rights reserved.)

A magnetic adsorbent (MA) was synthesized from wasted iron mud of a groundwater treatment plant using a novel one-step hydrothermal method. The results showed that Fe content of MA was 41.8 wt%, 2.5 times higher than that of iron mud, which was caused by hydrothermal dissolution of non-ferrous impurities under alkaline condition, such as quartz and albite, regardless of addition of ascorbic acid or not. Ferrihydrite was 92.7% in dry iron mud before adding ascorbic acid and gradually decreased to 58.1% by increasing the molar ratio of ascorbic acid to Fe following hydrothermal treatment. The strongest saturation magnetization of 16.29 emu/g was observed in the prepared MA-4 when the ascorbic acid to Fe molar ratio was 1. The highest surface site concentration of 1.31 mmol/g was observed in MA-2 when the ratio was 0.02. The mechanism of hydrothermal conversion of wasted iron mud to MA was reductive dissolution of ferrihydrite to form siderite, which was then reoxidized to maghemite. When 12.5 g/L of MA-2 was applied to treat smelting wastewater, over 99% removal of Cu 2+ , Zn 2+ , Pb 2+ , and Cd 2+ was achieved. The major mechanisms of Cu 2+ and Zn 2+ adsorption by the adsorbent were cationic exchange.

Chloride ion (Cl - ) is one of the most common anions in the aqueous environment. A mathematical model was developed to determine and quantify the impact of Cl - on the oxidization rate of organic compounds at the beginning stage of the UV/persulfate (PS) and UV/H 2 O 2 processes. We examined two cases for the UV/PS process: (1) when the target organic compounds react only with sulfate radicals, the ratio of the destruction rate of the target organic compound when Cl - is present to the rate when Cl - is not present (designated as r R Cl - / r R ) is no larger than 1.942%; and (2) when the target organic compounds can react with sulfate radicals, hydroxyl radicals and chlorine radicals, r R Cl - / r R , can be no larger than 60%. Hence, Cl - significantly reduces the organic destruction rate in the UV/PS process. In the UV/H 2 O 2 process, we found that Cl - has a negligible effect on the organic-contaminant oxidation rate. Our simulation results agree with the experimental results very well. Accordingly, our mathematical model is a reliable method for determining whether Cl - will adversely impact organic compounds destruction by the UV/PS and UV/H 2 O 2 processes.

The increasing number of applications in which copper oxide nanoparticles (CuO NPs) are used, may lead to potential release of CuO NPs into the environment. However, the impact of natural organic matters on the behavior and fate of CuO NPs in aquatic media is still largely unknown. In this study, the dissolution and aggregation of CuO NPs under the exposure of tannic acid (TA) were monitored over a period of 72 h, with a focus on assessing the contributions of solution pH changes and complexation reactions. Results showed that the total amount of Cu 2+ released from CuO NPs increased in the presence of TA especially at the highest TA concentration of 73.5 μmol/L. Although TA was observed to wrap around the CuO NPs, the aggregation of CuO NPs was not strongly influenced by TA and by the solution pH as investigated in this study. The kinetics of Cu 2+ release were fitted using the modified pseudo second-order model and the rate of dissolution was assessed to be highest at TA = 14.7 μmol/L. At pH = 4, the increased H + concentration was responsible for increased Cu 2+ release, whereas the complexation reaction between Cu 2+ and TA dominated at pH = 7. These findings suggested that the effects of TA on the dissolution of CuO NPs were a combination of solution pH change and complexation reaction, the relative fractions of which also depended on the solution pH. Additionally, the percentage of Cu 2+ released from the CuO NPs was found to increase upon decreasing concentrations of CuO NPs. Our work helps to further understand how and to which extent natural organic matters affect the behavior and fate of CuO NPs., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

Controlled-release KMnO4 (CRP) technology has been recently developed as an improved, highly efficient technique in wastewater treatment. In this study, batch-style experiments were conducted to evaluate this technology. The release characteristics of CRP in distilled water and the reaction between CRP and phenol were studied and fitted using MATLAB software. Results indicated that in distilled water, temperature (T) and pH value had a larger effect than dissolved oxygen (DO) concentration on the release characteristics of KMnO4, and this relationship can be accurately described by the following kinetic equation: logQ = log[1.141T(0.152)(pH)(-1.0536)(DO)(0.4674)] + [0.0048T(0.3756)(pH)(1.8854)(DO)(-0.0509)]logt. KMnO4 released from CRP can effectively degrade phenol-contaminated water with different concentrations. A simulated equation (r = -dCA/dt = -15.1705 CA(0.6840)CP(-0.1406)) characterizing phenol degradation was developed using MATLAB software. Comparison between the theoretical phenol removal rates deduced by the above two equations and the initial phenol concentration as well as the CRP dosage with the experimental data indicates that the differences between them were less than 20%. The results indicate phenol can be effectively removed by CRP and smaller dosage of KMnO4 was required compared with literature values. The models can provide guidance for CRP application in real polluted sites, which can lower the cost for site remediation.

A novel intimate integrated flocculation-adsorption fluidized bed (IFAFB) was designed based on the hydraulic classification theory, and the operation, performance, characterization, and mechanisms of the novel process were developed. In this system, 150 mg · L(-1) kaolin clay and 100 mg · L(-1) phenol were used to simulate multi-pollutants in synthetic influent; resin beads and silica beads were the solid phases for the fluidized flocculator, and polymer aluminum chloride (PAC) and granular activated carbon were the flocculant and the adsorbent, respectively. The results showed that the Euler numeral was the most suitable dynamic parameter for flocculation in the fluidized bed when compared with the velocity gradient (G), Reynolds number (Re), and GRe (-1/2) . Additionally, the adsorption capacities of the fluidized regime were 8.77 and 24.70 mg · g(-1) greater than those of the fixed regime at superficial velocities of 6 and 8 mm · s(-1), respectively. In the IFAFB, the removal efficiencies of kaolin clay and phenol in the IFAFB reached 95 and 80 % simultaneously at total initial bed height of 35 mm. Flocs size, fractal dimension, and scanning electron microscopy (SEM) confirmed that the relationship of flocculation and adsorption in the IFAFB was mutually beneficial. Adsorption favored continuous growth of flocs and protected flocs from breakage, while flocculation removed fine particles as the first stage to prevent the adsorption of kaolin clay.

A fluidized bed photoreactor with titanium dioxide-immobilized spherical activated carbon particles was examined. The light intensity profile was modeled using the Lambert-Beer rule for the modeling of the radial distribution of liquid-phase phenol concentration in the fluidized bed photoreactor, when considering the reactor composed of numerous differential annular drums and no mass transfer between drums. The model could be well matched with the experimental data which indicated the liquid flow rate of 13.8 L/min was the optimum in the balance of flow rate-related light penetration and photocatalyst concentration. By integration of liquid-phase phenol concentration along the radius, photocatalytic oxidation performance of the photoreactor was evaluated in comparison with the experimental data and model prediction. The results showed that the errors were less than 30% for most of the predictions. It is suggested that mass transfer and flow rate difference along the radial direction should be considered to obtain more precise prediction.