ENVIRONMENTAL POLLUTION
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2022
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IF 9.988
Liuyang He,Shangding Yang,Lie Yang,Shitai Shen,Yulong Li,Dejin Kong,Zhuqi Chen,Shengmao Yang,Jia Wang,Li Wu,Zulin Zhang
The non-radical pathway of periodate (PI) activation for the removal of persistent organic contaminants has received increasing attention due to its higher stability and oxidative advantages. In this study, the degradation of sulfamethoxazole (SMX) by ball mill treated magnetic sludge biochar (BM-MSBC) through activation of PI by electron transfer mechanism was reported. Experimental and characterization results showed that the ball milling treatment resulted in a better pore and defect structure, which also significantly enhanced the electron transfer capacity of the sludge biochar. The BM-MSBC/PI system exhibited notable dependence of activator concentration and initial pH, while the effect of PI concentration was not significant. The coexisting substances (common anions and natural organic matters) hardly affect the degradation of SMX in the BM-MSBC/PI system. The phytotoxicity experiments suggested that the treatment of BM-MSBC/PI system could significantly reduce the biological toxicity of SMX solution. This study provides a novel, economical, and facile modification method for the application of sludge biochar in advanced oxidation processes .
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Shizong Wang,Haiyang Liu,Jianlong Wang
In this study, nitrogen, sulfur and oxygen co-doped carbon armored cobalt sulfide (Co/Co 9 S 8 @N-S-O-C) composite was synthesized, characterized and used to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX). SMX (0.04 mM) can be completely degraded within 20 min in the presence of 0.8 mM PMS and 0.1 g/L Co/Co 9 S 8 @N-S-O-C composite. The first-order kinetics constant of SMX degradation was 0.307 min -1 , and the mineralization of SMX was 30.1 %. The Quenching experiments of the free radicals and the identification of degradation products demonstrated that sulfate radicals played a dominant role in SMX degradation. The degradation rate of SMX increased with temperature, and activation energy was calculated to be 48.6 kJ/mol. The degradation rate of SMX increased firstly then decreased with increase of pH. Chloridion and humic acid decreased the degradation rate of SMX no matter what their initial concentration was. The effect of carbonate on SMX degradation depended on its initial concentration. Co/Co 9 S 8 @N-S-O-C composite showed good stability, the removal efficiency of SMX was 98.4 % in the fifth experiment. Based on the characterization results of the catalyst before and after use, it was concluded that cobalt, sulfur, pyridnic N and graphitic N were responsible for PMS activation.
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PubMed
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2023
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IF 8.7
Feiyu Zhang,Shuqian Cheng,Jinbo Zhao,Anjie Li
Even after pre-treatment, livestock and poultry wastewater still contain high concentrations of ammonia and residual antibiotics. These could be removed economically using the aerobic granular sludge (AGS) process with zero-valent iron (ZVI). The interaction of antibiotics and nitrogen in this process needs to be clarified and controlled, however, to achieve good removal performance. Otherwise, antibiotics might generate transformation products (TPs) with higher toxicity and lead to the emergence of antibiotic-resistant bacteria carrying antibiotic resistance genes (ARGs), which could cause persistent toxicity and the risk of disease transmission to the ecological environment. This study investigated the impact of ZVI on AGS for nitrogen and sulfamethoxazole (SMX) removal. The results show that AGS could maintain good ammonia removal performance and that the existence of SMX had a negative impact on ammonia oxidation activities. ZVI contributed to an increase in the abundance of nitrite oxidation bacteria, denitrifying bacteria and the functional genes of nitrogen removal. This led to better total nitrogen removal and a decrease in N 2 O emission. Accompanied by biological nitrogen transformation, SMX could be transformed into 14 TPs through five pathways. ZVI has the potential to enhance transformation pathways with TPs of lower ecotoxicity, thereby reducing the acute and chronic toxicity of the effluent. Unfortunately, ZVI might enhance the abundance of sul1 , sul2 , and sul3 in AGS, which increases the risk of sulfonamide antibiotic resistance. In AGS, Opitutaceae , Xanthomonas , Spartobacteria and Mesorhizobium were potential hosts for ARGs. This study provides theoretical references for the interaction of typical antibiotics and nitrogen in the biological treatment process of wastewater and bioremediation of natural water bodies.
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PubMed
高影响因子
ANALYST
·
2023
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IF 4.2
Mingjiao Shi,Peizheng Shi,Xinxin Yang,Ningbin Zhao,Mengfan Wu,Jing Li,Chen Ye,He Li,Nan Jiang,Xiufen Li,Guosong Lai,Wan-Feng Xie,Li Fu,Gang Wang,Yangguang Zhu,Hsu-Sheng Tsai,Cheng-Te Lin
The presence of sulfamethoxazole (SMX) in natural waters has become a significant concern recently because of its detrimental effects on human health and the ecological environment. To address this issue, it is of utmost urgency to develop a reliable method that can determine SMX at ultra-low levels. In our research, we utilized PVP-induced shape control of a hydrothermal synthesis method to fabricate layer-like structured VS2, and employed it as an electrode modification material to prepare an electrochemical sensor for the sensitive determination of SMX. Thus, our prepared VS2 electrodes exhibited a linear range of 0.06–10.0 μM and a limit of detection (LOD) as low as 47.0 nM (S/N = 3) towards SMX detection. Additionally, the electrochemical sensor presented good agreement with the HPLC method, and afforded perfect recovery results (97.4–106.8%) in the practical analysis. The results validated the detection accuracy of VS2 electrodes, and demonstrated their successful applicability toward the sensitive determination of SMX in natural waters. In conclusion, this research provides a promising approach for the development of electrochemical sensors based on VS2 composite materials.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Le Chen,Min Wang,Qian Sun,Zhongbao Zhao,Jiangang Han,Rongting Ji,Xin Jiang,Yang Song,Jianming Xue,Hu Cheng
Efficient sorbents that have high sorption capacity and suitable separability are promising and are urgently needed to remove diverse contaminants from water environments. In this study, nitrogen-doped magnetic porous biochars (NMPBs) were synthesized from marine algae by a three-step process consisting of prepyrolysis, copyrolysis and coprecipitation. For NMPBs, the surface area was up to 1531 m 2 /g, the magnetization strength was up to 31 emu/g, and the surface nitrogen content was up to 3 %. The NMPBs showed the expected sorption capability for sulfamethoxazole, with the removal quantity reaching 502 mg g −1 based on the sorption isotherm model. NMPBs also showed excellent separability and reusability, and the removal rate remained at 87 % after seven cycles. Partitioning and adsorption, including pore filling, hydrogen bonding, π-π stacking, partitioning and electrostatic interactions, were the sorption processes in removing sulfamethoxazole. In this work, marine algae were converted into an engineered biochar that is promising for environmental remediation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Amina,Xiongyuan Si,Kang Wu,Youbin Si,Balal Yousaf
In this study, a modified Fenton system using calcium peroxide (CaO 2 ) powder, as an effective source of hydrogen peroxide (H 2 O 2 ), for the degradation of sulfamethoxazole (SMX) in aqueous solution was investigated. Our results indicated that degradation of SMX in Fe(II)-EDTA catalyzed CaO 2 system was readily more efficient than in Fe(II) catalyzed CaO 2 system. The SMX degradation efficiency was found maximum at pH 6.0 and SMX degradation was suppressed as the initial solution pH was increased. Nevertheless overall removal efficiency in this system was favorable near to neutral pH. In addition, it was observed that the higher bicarbonates (HCO 3 − ) contents had a considerable scavenging ability to SMX degradation while low concentration exhibited auspicious role. The presence of chlorides (Cl − ), nitrates (NO 3 − ), sulfates (SO 4 2− ), and humic acid (HA) could improve SMX removal in this Fenton-like system. Furthermore, chemical probe and radical scavenging activity confirmed the formation of hydroxyl (HO ) and superoxide (O 2 − ) radicals, and also described that the SMX degradation was predominantly due to the HO -induced oxidative destruction. Electron paramagnetic resonance (EPR) studies for different systems, different pH values and different reaction times were carried out to determine the HO radical intensities. EPR results showed that HO intensities were higher in Fe(II)-EDTA catalyzed CaO 2 system, at pH 6.0 and at 90 s reaction time, respectively. Intermediate products of SMX were identified and possible mechanism of SMX degradation was suggested. In conclusion, this work provided comprehensive knowledge for the use of Fe(II)-EDTA catalyzed CaO 2 system for remediation of SMX contaminated sites.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Wenqi Wang,Ming Chen
Nitrogen doping could improve the catalytic performance of carbon materials, in which the nitrogen configuration could be used as active sites for peroxymonosulfate (PMS) activation. Herein, this paper studied how to turn waste to “treasure” by agriculture waste pomelo peel to prepare nitrogen-doped biochar and successfully applied it to advanced oxidation field. The effects of the sodium bicarbonate (NaHCO 3 ), melamine, and pyrolysis temperature on the catalytic activity of biochar for the removal of sulfamethoxazole (SMX) were investigated. The optimized nitrogen-doped biochar (C−N−M 1:3:4) possessed high specific surface area (SSA, 738 m 2 /g) and high level of nitrogen doping (nitrogen content 13.54 at%). Accordingly, it exhibited great catalytic performance for PMS activation to remove SMX antibiotic, and 95% of SMX was removed within 30 min. High catalytic activity of C−N−M 1:3:4 was attributed to rich defects, carbonyl group, high content of graphitic N and pyrrolic N, and large SSA, in which non-radical oxidation process based on singlet oxygen ( 1 O 2 ) and electron transfer contributed to the SMX degradation. The prepared nitrogen-doped biochar possessed high stability and reusability and the removal efficiency of SMX still reached 80% after four cycles. Additionally, the phytotoxicity assay indicated that the toxicity of degradation intermediates was obviously decreased in the PMS/ C−N−M 1:3:4 system.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Shuyi Shen,Tao Ke,Dike Fang,Daohui Lin
Visible-light-driven photocatalysts with synergistic persulfate (PS) activation and photocatalysis possess enormous pollution-control potential. Herein, nitrogen and sulphur co-doped TiO 2 @C hybrid (N/S-TiO 2 @C) featuring the complementary visible-light photocatalysis and synergetic PS activation was synthesized by in situ oxidation of Ti 3 C 2 MXene and thereafter co-doping with N and S. Both anatase and rutile phases of TiO 2 were attained in N/S-TiO 2 @C. The decrease of TiO 2 bandgap (about 1.81 eV) and the defect of carbon layer caused by the N and S co-doping in both TiO 2 crystal and carbon layer enabled the synergistic enhancement of PS activation and photocatalysis. Complete degradation and 93.4% mineralization of sulfamethoxazole (SMZ, 10 mg/L) were achieved by dosing PS (2 mM) and N/S-TiO 2 @C (0.4 g/L) under visible light within 30 min. The degradation rate by N/S-TiO 2 @C through PS activation under visible light was 27.9-, 11.1-, and 2.30-fold higher than that by PS, N-TiO 2 @C, and S-TiO 2 @C alone, respectively. Reactive species SO 4 − , 1 O 2 , OH, and O 2 − , especially the former two, were determined dominating the SMZ degradation, and the degradation pathways were illustrated through intermediates identification. Moreover, N/S-TiO 2 @C kept excellent performance in activating PS to degrade SMZ in real water samples. These results indicate that N/S-TiO 2 @C is a stable and promising PS activator under visible light and has a good application potential in organic wastewater treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yu Jiang,Jia Wang,Bo Liu,Wei Jiang,Tianyu Zhou,Yunchao Ma,Guangbo Che,Chunbo Liu
Herein, a N,S,O-doped Co/CoO/Co 9 S 8 @carbon hybrid (Co/CoO/Co 9 S 8 @NSOC) has been constructed by calcinating a Co-based metal–organic framework (Co-MOF) with 4,4-bipyridine and 2,5-thiophenedicarboxylic acid as linkers. Co/CoO/Co 9 S 8 @NSOC exhibited a high and recycled catalytic efficiency for peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX, 20 mg/L) with a reaction rate of 1.31 min −1 , which was 5.2 times than that of Co-MOF. The catalytic behavior should be attributed to the rich active sites, lamellar morphology, superhydrophilicity, and magnetism. Furthermore, the Co/CoO/Co 9 S 8 @NSOC was immobilized on a filter membrane (CMFM) to adapt to the flowing system, which could recycle 20 times without losing activity. To employ in a large-scale static environment, the Co/CoO/Co 9 S 8 @NSOC was loaded on the commercial sponge (CoSPG). In a 50 L water tank, the CoSPG realized to decompose 160 mg/L SMX solution with 37 h and had long-term stability over 10 days. Notably, the PMS cost of treating one ton of wastewater is only $0.34, indicating a huge industrial application value.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Amina,Xiongyuan Si,Kang Wu,Youbin Si,Balal Yousaf
In this study, fabrication of manganese-incorporated iron oxide-graphene nanocomposite (rGO-FMBO) was reported for the efficient activation of CaO 2 and generation of reactive radicals for the degradation of sulfamethoxazole (SMX). The effects of different systems, catalyst dosage, oxidant dosage, different pH and different reaction time on the degradation of SMX by rGO-APTMS-FMBO/CaO 2 as well as the production of free radicals were also studied. Electron paramagnetic resonance (EPR) technique was used to detect and identify the radical species in this oxidation system and these radicals were further confirmed by scavenging studies with the addition of isopropanol (IPA) and methyl viologen (MV 2+ ). The results indicated that the CaO 2 could be activated by rGO-APTMS-FMBO efficiently for the effective degradation of SMX at neutral pH ( P ≤ 0.01). The mechanism of the activation of CaO 2 by rGO-APTMS-FMBO was that carbon dioxide radicals (CO 2 − ) generated by rGO-APTMS-FMBO could activate the CaO 2 to produce more hydroxyl radicals (HO ), which favored the SMX degradation. EPR studies showed that three types of free radicals HO , CO 2 − , and CH 3 were generated and the radical intensities were much higher in rGO-APTMS-FMBO/CaO 2 system. Both increased pH and reaction time led to the production of more CO 2 − , which activated the CaO 2 to give more HO to degrade SMX. Transformation products/intermediates of SMX were determined and potential mechanism and degradation pathway were proposed. The findings of this study provide new insights into the mechanism of heterogeneous catalysis based on CaO 2 activated by rGO-APTMS-FMBO and the reactivity of this oxidation system toward environmental contaminants.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Zhikang Deng,Yongfei Ma,Jinyao Zhu,Chenyu Zeng,Rui Mu,Yifan Liu,Ping Li,Zulin Zhang
Ferrate (Fe (VI)), as a versatile oxidizer, has been widely employed for water treatment. However, the rapid self-decomposition of Fe (VI) diminishes its practical application efficiency. In this study, a novel Mn-modified sludge biochar (MSBC) was synthesized for the first time to activate Fe (VI) and generate highly reactive Fe (IV)/Fe (V) for the rapid removal of sulfamethoxazole (SMX). The results showed that MSBC (0.10 g/L) effectively activated Fe (VI) (100 μM), and 87.39 % of SMX (10 μM) and 40.26 % of total organic carbon (TOC) were removed within 10 min. Notably, raising the solution pH (e.g., from 6.0 to 11.0) would result in decreasing the reactivity of Fe (VI) and a lower removal efficiency of SMX. The quenching, electron paramagnetic resonance and probe experiments suggested that •O 2 – and high-valent iron species (Fe (V)/Fe (IV)) were identified as the major contributions to the removal of SMX. The detailed activation sites of MSBC were –OH and Mn-O, as corroborated by density functional theory (DFT) calculation and characterization. These activation sites facilitated activation of Fe (VI) through efficient electron transfer . The Fukui index indicated that the N, S, and O atom of SMX were the primary attacked sites. Subsequently, five potential degradation pathways were proposed, with the cleavage of the S-N bond being the predominant one. The toxicity of these products was examined using ECOSAR program, revealing that main products showed low toxicity or non-toxicity. The Cl - , SO 4 2- , and NO 3 – had negligible effect on SMX degradation, although excessive concentrations of HCO 3 – and humic acid (HA) showed slightly inhibition. Additionally, the Fe (VI)/MSBC system also effectively removed 87.34 % of sulfadiazine (SDZ) and 93.91 % of sulfamethoxypyridazine (SMP). Overall, this study offered a practical and cost-effective approach for the activation of Fe (VI) and provided new insights to the degradation mechanism.
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高影响因子
WATER RESEARCH
·
2022
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IF 13.4
Ai Zhang,Yongquan Zhou,Yongmei Li,Yanbiao Liu,Xiang Li,Gang Xue,Andere Clement Miruka,Ming Zheng,Yanan Liu
Large amounts of antibiotics are concentrated in waste activated sludge (WAS) and released into the environment. It is thus critical to develop advanced sludge treatment technology to remove these antibiotics. Dielectric barrier discharge (DBD) combined with calcium peroxide (CaO 2 ), as an innovative technology to attenuate sulfamethoxazole (SMX) in sludge, was investigated. Evident synergistic effects between DBD and CaO 2 were observed on the SMX degradation with a synergistic factor of 2.02. Moreover, the energy consumption of DBD/CaO 2 was significantly lower than that of DBD alone. At a typical CaO 2 dosage of 0.1 g/g TS and discharge power of 64.5 W, the highest SMX removal of 96% was achieved within 50 min. The synergistic effects of DBD/CaO 2 could be associated with the base catalysis of H 2 O 2 and O 3 , UV-base-photolysis, peroxone oxidation, and photocatalytic H 2 O 2 . DBD/CaO 2 generated various reactive oxygen species (ROS) and nitrogen species (RNS) that participated in SMX removal. The contributions of these reactive species followed the sequence of e − > •OH > •O 2 − > 1 O 2 > ONOO − . Based on the detected transformation by-products and their variations during treatment, a plausible SMX degradation pathway in sludge was proposed. Besides, DBD/CaO 2 also promoted sludge disintegration, dewatering, heavy metal removal, sludge reduction, sludge solubilization, and acetate-enriched volatile fatty acid (VFA) production. Therefore, DBD/CaO 2 exhibited great potential for controlling antibiotic, as well as promoting sludge reduction, decontamination, and resourcization.
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高影响因子
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