JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Wenxin Shi,Qingjie Li,Rongqing Qi,Heli Tang,Bing Zhang
Aerobic granular sludge membrane system (AGSMS) represents a new wastewater reuse treatment technology. However, the challenges of membrane fouling and limited micropollutant removal efficiency significantly impact its potential for further application. Consequently, this study aimed to address these concerns by employing Fe 3 S 4 /persulfate pretreatment to mitigate membrane fouling and enhance perfluorooctanoic acid (PFOA) removal in AGSMS. The effects of pH and persulfate types were investigated by assessing membrane flux, fouling resistance, membrane characterization, and effluent properties. Results showed that optimal mitigation of membrane fouling and removal of PFOA were achieved using Fe 3 S 4 -activated PMS at a pH of 6. The primary mechanism for Fe 3 S 4 -activated PMS involved the generation of SO 4 •− and 1 O 2 . Moreover, the fouling mechanism transitioned from cake layer fouling and intermediate blocking fouling to complete blocking fouling in the presence of Fe 3 S 4 /PMS. The application of extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory revealed that at pH 6.0, there was a significant increase in the energy barrier for both foulant-membrane and foulant-foulant interactions, leading to an effective mitigation of membrane fouling. Correlation analysis demonstrated a significant influence of polysaccharides and total phosphorus concentration on mitigating membrane fouling. Furthermore, pH played a crucial role in mitigating membrane fouling as well as pollutant removal by influencing both coexisting ion states in solution and catalyst properties. This study offers valuable insights for future research and provides essential theoretical guidance for large-scale applications of AGSMS technology in wastewater treatment .
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Yuhang Zhang,Donglei Li,Liang She,Furong Guo,Falong Jia,Lizhi Zhang,Zhihui Ai,Xiao Liu
Heavy metal complexes in industrial wastewater are challenging to be removed by conventional methods arising from their stable chelating structure. In this study, zero-valent iron (ZVI) was ball-milled with tiny formic acid (FA), and the as-prepared sample (FA-ZVI bm ) was attempted to eliminate a model heavy metal complex of Cu(II)-ethylenediaminetetraacetic acid (Cu(II)-EDTA). The addition of FA to ball-milling could dramatically enhance the performance of ball-milled ZVI (ZVI bm ) towards Cu(II)-EDTA removal and increase the removal rate constant by 80 times. This conspicuous improvement of Cu(II)-EDTA elimination was attributed to the ferrous formate (Fe(HCOO) 2 ) shell formed on the surface of FA-ZVI bm . Results revealed that the Fe(HCOO) 2 shell facilitated the activation of O 2 to reactive oxygen species (ROS) and the leaching of Fe 3+ . Cu(II)-EDTA was decomplexed through both oxidative destruction and Fe 3+ replacement, and the released Cu 2+ was reduced by FA-ZVI bm and immobilized synchronously. Meanwhile, the ligands underwent oxidative degradation by ROS, thus avoiding the re-chelation ecological risk. Impressively, FA-ZVI bm could achieve cyclic treatment of actual copper complex wastewater and possessed promising advantage in treatment cost. This study would offer a promising approach for eliminating Cu(II)-EDTA through EDTA ligands degradation and synchronous Cu(II) removal, moreover to shed light on the decomplexation mechanism.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Le Zhang,Ting Liu,Meng Zhu,Yong Liu
Persulfate (PS)-based advanced oxidation processes (SR-AOPs) is a promising approach for the removal of ammonia nitrogen (NH 3 -N) from wastewater, but it suffered from the low removal efficiency and the excessive oxidation of NH 3 -N to nitrate (NO 3 − ) or nitrite (NO 2 − ) in the absence of in-situ generated chlorine radicals. Therefore, it is still a challenge to improve the efficiency of NH 3 -N removal and the selectivity of NH 3 -N oxidation products towards dinitrogen (N 2 ) by SR-AOPs without chlorine radicals. Herein, a novel photo-assisted activation of SR-AOPs involving sodium silicate (Na 2 SiO 3 ) and sodium sulfite (Na 2 SO 3 ) was developed for NH 3 -N removal from wastewater. In this system, Na 2 SiO 3 was acted as a green buffer to maintain NH 3 -N in the form of un-ionized ammonia (NH 3 ) with strong reducibility, promoting the efficiency of NH 3 -N removal as well as ensuring the neutral effluent by receiving the H + from PS activation. Na 2 SO 3 could inhibit the excessive oxidation of NH 3 -N by regulating the redox potential of the solution and generating hydrated electrons (e aq − ) under light ( hv) irradiation, enhancing the selectivity of NH 3 -N oxidation products towards N 2 . 100 % of NH 3 -N removal efficiency and more than 98 % of N 2 selectivity were obtained after 30 min at the initial pH of 3–9 and the initial NH 3 -N concentration of 30 mg N/L. Based on the quenching experiment, EPR test and probe experiment, the HO and SO 4 − were the main reactive oxygen species (ROS) to be responsible for NH 3 -N oxidation. This study proposed a new approach for treatment of wastewater containing NH 3 -N by SR-AOPs.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Shilong Jiang,Song Cheng,Jiashun Cao,Cailiang Yue,Jianglei Xiong,Cong Jiang,Hongzhan Cai,Jianhua Wu
The removal of trace urea presents a significant challenge in the production of electronic-grade ultra-pure water (UPW). This study proposed a simple strategy to regulate the low-coordination of a single-atom cobalt catalyst (R y Co-CN 0.20 ) for the efficient removal of trace urea via peroxymonosulfate (PMS) activation. The optimal R 0.50 Co-CN 0.20 with low-coordination Co-N 3 sites was constructed by in-situ reduction of NaBH 4 and significantly enhanced the PMS activation. The removal efficiency of trace urea achieved 94 % within 5 mins. The k obs of trace urea degradation in R 0.50 Co-CN 0.20 /PMS system reached 0.4576 min −1 , which was much higher than previous reported systems. Experiments of free radical quenching and electron paramagnetic resonance demonstrated that singlet oxygen species were the dominant free radical. The corresponding steady concentration of singlet oxygen species in the R 0.50 Co-CN 0.20 /PMS system was enhanced to be 16.361 × 10 –6 μM, which was twice of Co-CN 0.20 /PMS. Density functional theory calculations revealed that the optimized electron distribution of the Co center in the Co-N 3 sites processed a higher d band center (−1.08 eV) and richer electron transfer number (0.75 e − ) compared with Co-N 4 sites, hence realizing the stronger PMS activation. Continuous operation verified that R 0.50 Co-CN 0.20 /PMS could maintain the removal rate of trace urea above 80 % after 150 h operation. Moreover, R 0.50 Co-CN 0.20 /PMS in the pilot UPW production process effectively reduced the pollution caused by trace urea and ensured the quality of the terminal UPW (Total organic carbon <1 μg/L). This study provides a new approach for the removal of trace urea through PMS activation by low-coordination single-atom catalysts.
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ENVIRONMENTAL RESEARCH
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2023
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IF 8.3
Jiamin Gong,Honghui Jiang,Xiang Li,Hao Cheng,Ziqi Wang,Jingju Cai,Meifang Li,Ping Wang,Hui Wang,Xi Hu,Xinjiang Hu
In this study, the manganese oxide/biochar composites (Mn@BC) were synthesized from Phytolacca acinosa Roxb. The Mn@BC was analyzed via techniques of Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and X-ray diffraction analysis (XRD). The results show that MnO x is successfully loaded on the surface of BC, and the load of MnO x can increase the number of surface functional groups of BC. X-ray photoelectron spectroscopy (XPS) shows that MnO x loaded on BC mainly exists in three valence forms: Mn(Ⅱ), Mn(Ⅲ), and Mn(Ⅳ). The ability of Mn@BC to activate periodate (PI) was studied by simulating the degradation of methylene blue (MB) dye. The degradation experiment results showed that the MB removal rate by the Mn@BC/PI system reached 97.4% within 30 min. The quenching experiment and electron paramagnetic resonance (EPR) analysis confirmed that Mn@BC can activate PI to produce iodate (IO 3 •), singlet oxygen ( 1 O 2 ), and hydroxyl radical (•OH), which can degrade MB during the reaction. Response surface methodology (RSM) based on Box-Behnken Design (BBD) was used to determine the interaction between pH, Mn@BC and PI concentration in the Mn@BC/PI system, and the optimum technological parameters were determined. When pH = 5.4, Mn@BC concentration 0.56 mg/L, PI concentration 1.1 mmol/L, MB removal rate can reach 98.05%. The cyclic experiments show that Mn@BC can be reused. After four consecutive runs, the removal rate of MB by the Mn@BC/PI system is still 82%, and the Mn@BC/PI system also shows high performance in treating MB in actual water bodies and degrading other pollutants. This study provides a practical method for degrading dyes in natural sewage.
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Journal of Water Process Engineering
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2023
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IF 7
Jiaqi Wei,Yuanyuan Zhang,Jinxing Ma,Shanshan Wang,Minmin Jiang,Qiaoyan Wei,Mei Chen,Xiaowu Huang,Haixiang Li,Xuehong Zhang,Junjian Zheng
Degradation of refractory organics has been limited by their low mass-transport rates in conventional flow-by operated electrochemical reactors. This study explores for the first time the development of porous titanium (Ti)-based metal oxide anodic membrane for efficient flow-through degradation of recalcitrant tetrabromobisphenol A (TBBPA). For this purpose, a duplexed Ti/SnO 2 -Sb/PbO 2 -Ce anodic membrane was successfully prepared by sol-gel and electrodeposition methods. Ti/SnO 2 -Sb/PbO 2 -Ce exhibited improved mechanical and electrochemical stability, larger electrochemical surface area, higher oxygen evolution potential and lower charge transfer resistance, as compared to its mono-layered rival (Ti/SnO 2 -Sb). The switching from flow-by to flow-through operation resulted in an increased mass transfer rate constant and narrowed diffusion layer thickness of Ti/SnO 2 -Sb/PbO 2 -Ce. In the flow-through mode, Ti/SnO 2 -Sb/PbO 2 -Ce enabled the complete TBBPA removal at a relatively low electric energy (0.11 kWh m −3 ). The TBBPA removal was ascribed to the direct anodic oxidation and indirect anodic oxidation incurred by absorbed HO , free HO and 1 O 2 . The intermediate products, which were arisen from the attack of TBBPA by these reactive species, were identified. We further estimated their acute toxicities and bioaccumulation factors. This research proposed a robust electrochemical filtration approach for detoxification of TBBPA-contaminated water.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Lei Xu,Le Liang,Chen Chen,Ze-Hang Chen,Zong-Bin Lv,Ming-Lai Fu,Baoling Yuan
The rapid accumulation of spent lithium-ion batteries (SLIBs) poses a global challenge in terms of their disposal and management. Considering the substantial quantity of transition metals contained in SLIBs, the preparation of derived catalysts for environmental remediation has emerged as a promising approach for the recycling of SLIBs. Herein, the citric acid-based sol-gel method was employed to synthesize the catalyst from SLIBs. The derived spent cathode material (LiNi x Co y Mn 1−x-y O 2 , NCM) composites exhibit superior catalytic activity and display higher adaptability to the environment, effectively removing typical azo dye, methylene blue (MB), as well as various organic contaminants , sulfamethoxazole (SMX), levofloxacin (LVF) and rhodamine B (RhB) in 30 min. The Co 2+ and Mn 2+ ions in the catalyst play a crucial role in activating PMS to generate 1 O 2 and O 2 •− . The degradation of MB proceeds through several reaction pathways, including demethylation, oxidation , and ring-opening reactions, as confirmed by the Fukui function and UPLC-QTOF-MS analyses. The assessment of toxicity in the degradation products was conducted using T.E.S.T. and ECOSAR 2.0. This proposed method can be highly suggested as a promising strategy for the recycling and utilization of SLIBs, transforming them into efficient catalysts for PMS systems in environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Junjie Zhang,Yongjia Hong,Xu Tang,Yong Chen,Wenran Gao,Yuncheng Cai,Ningning Dong,Jiazi Xu,Li Zhang,Quli Fan,Bin Sun
The rational design of active sites in nanocarbons are the long-term pursuit for their practical applications. However, N, as the most potential active site, still encounters the problems of low atom utilization efficiency and stability in practical environmental remediation. Herein, we successfully constructed synergistic active sites consisting of graphitic N, pyridinic N, and thiophene S in heavy S, N co-doped hollow graphene spheres (HSNGS). The HSNGS exhibited exceptional efficiency in degrading tetracycline in real water, with a turnover frequency of 6.24 min −1 , which is among the highest reported. Moreover, tetracycline dissolved in practical water could be continuously and rapidly eliminated by passing through a column filled with HSNGS, maintaining its high performance even after 40 consecutive cycles. In the synergistic active sites, graphitic N and pyridinic N species accepted electrons from peroxymonosulfate, generating singlet oxygen for tetracycline degradation. Simultaneously, thiophene S coordinated with metal ions present in the practical water, synergistically enhancing the degradation of tetracycline. Additionally, the coordinated metal ions provided protection for the synergistic active sites during peroxymonosulfate activation, preventing their oxidation and enabling the continuous and rapid degradation of tetracycline. This work opens up possibilities for the industrial application of nanocarbon materials in environmental remediation.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Danni Cui,Huan He,Wenxiao Xie,Shanshan Yang,Ziwei Guo,Zhicheng Liao,Feng Liu,Chaochao Lai,Xiaomin Ren,Bin Huang,Xuejun Pan
17α-ethinylestradiol (EE2), a synthetic endocrine-disrupting chemical, can degrade in natural waters where humic acids (HA) and dissolved iron (DFe) are present. The iron is mostly bound in Fe(III)-HA complexes, the formation process of Fe(III)-HA complexes and their effect on EE2 degradation were explored in laboratory experiments. The mechanism of ferrihydrite facilitated by HA was explored with results indicating that HA facilitated the dissolution of ferrihydrite and the generation of Fe(III)-HA complexes with the stable chemical bonds such as C-O, C O in neutral, alkaline media with a suitable Fe/C ratio. 1 O 2 , •OH, and 3 HA* were all found to be important in the photodegradation of EE2 mediated by Fe(III)-HA complexes. Fe(III)-HA complexes could produce Fe(II) and hydrogen peroxide (H 2 O 2 ) to create conditions suitable for photo-Fenton reactions at neutral pH. HA helped to maintain higher dissolved iron concentrations and alter the Fe(III)/Fe(II) cycling. The natural EE2 photodegradation pathway elucidated here provides a theoretical foundation for investigating the natural transformation of other trace organic contaminants in aquatic environments.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2023
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IF 8.7
Zhengjie Peng,Shikai Li,Hao He,Yujiao Wen,Haolong Huang,Lezhu Su,Zhigang Yi,Xing Peng,Nan Zhou
Advanced oxidation processes (AOPs), based on sulfate radical (SO 4 ·- ) produced by peroxymonosulfate (PMS), can effectively mineralize refractory organic pollutants. However, the coexistence of anions and natural organic matters in actual wastewater prevents the application of AOPs. A simple one-step method was used to prepare FeS/Fe 3 O 4 co-modified biochar materials (FFB) that could activate PMS to degrade quinclorac (QNC) with a removal rate of 100%, even exhibiting optimum degradation of QNC reached 99.31% in irrigation water, demonstrating excellent anti-interference performance for co-existing anions and natural organic matter. Meanwhile, ecotoxicity analysis showed that the toxicity of degradation intermediates was lower than that of QNC. Characterization results demonstrated the even distribution of FeS and Fe 3 O 4 onto biochar, supplying abundant Fe 2+ to activate PMS producing reactive oxygen species (ROS), while the generated Fe 3+ after reactive continue to be reduced with sulfur species to promote the cycle of Fe 2+ /Fe 3+ . The coexistence of ·OH, SO 4 ·- , 1 O 2, and O 2 ·- in the FFB/PMS-QNC system suggest the possession of two pathway with free radical and non-free radical pathways to degrade QNC. The density functional theory (DFT) was used to analyze the adsorption sites and adsorption energy of PMS, as well as the differential charge density, which further proved the generation of SO 4 ·- , O 2 ·- and 1 O 2 . In addition, the electrochemical test results showed that electron transfer also played an important role in the degradation of QNC. This study provides a feasible approach for the removal of organic pollutants in actual water.
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WATER RESEARCH
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2023
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IF 12.8
Jialiang Liang,Jingke Wu,Pengfei Gan,Yudan Liu,Peng Zhen,Yunyi Li,Zhiwei Zhao,Wen Liu,Meiping Tong
Organophosphorus pesticides are extensively utilized worldwide, but their incomplete dephosphorization poses significant environmental risks. This study investigates the dephosphorization of dimethoate (DMT), a representative organophosphorus pesticide, using a vacuum ultraviolet system. Surprisingly, in addition to hydroxyl radicals ( • OH), non-radical processes such as photoexcitation and singlet oxygen atoms (O( 1 D)) exert more significant effects on DMT dephosphorization. The degradation kinetics of DMT demonstrate a perfect linear correlation with the radical yield in both UV-based and VUV-based advanced oxidation processes (AOPs), with greater efficacy of radical attack observed in the VUV system. This heightened efficiency is attributed to the excitation of DMT to a high-energy excited state induced by UV 185 radiation. Additionally, • OH alone is inadequate for achieving complete dephosphorization of DMT. The Fukui index and singly occupied orbital (SOMO) analysis reveal that the O( 1 D) generated by UV 185 -induced photolysis of O 2 exhibits exceptional selectivity towards P=S bonds, thereby playing an indispensable role in the dephosphorization process of DMT. This study highlights the significant contribution of non-radical pathways in DMT dephosphorization by VUV, which holds great implications for the advancement of photochemical-based AOPs.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Jun Hu,Ruiqi Wang,Shangkun Li,Jun Wu,Zhimin Qiang
Peroxymonosulfate (PMS) is an alternative disinfectant for drinking water . This study aimed to investigate the transformation of iopamidol (IPM) catalyzed by a main copper corrosion product ( c -Cu 2 O) with PMS as a disinfectant. The observed pseudo-first-order constant ( k obs ) for the IPM degradation in the c -Cu 2 O/PMS system (0.033 min −1 ) was 3 times that in the CuO/PMS system (0.011 min −1 ). The quenching tests and the electron paramagnetic resonance (EPR) experiments indicate that O 2 •− and 1 O 2 contributed to IPM degradation in the c -Cu 2 O/ PMS system. The complexation of metastable Cu(II) with a PMS molecule polarized the O O bond and then facilitated the electron transfer from the PMS molecule to other PMS and O 2 molecules, which directly and indirectly promoted the yield of O 2 •− and 1 O 2 . The iodine balance indicated that 26.0% of initial TOI was converted to IO 3 − , and CHI 3 only accounted for 0.6% of the residual TOI. In the c -Cu 2 O/PMS system, IPM conversion was started with amide C−N bond breakage, deiodination reaction and hydrogen abstraction. This study helps to better understand the conversion mechanisms of iodine-containing organic micropollutants when PMS is deployed as a disinfectant in copper pipes.
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