SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Bo Qin,Bin Wang,Jiang Li,Tao Wang,Xiaoyi Xu,Li'an Hou
Non-radical catalytic oxidation processes can eliminate refractory pollutants from wastewater containing complex substrates such as dissolved organic matter, but the production of selective non-radicals is challenging during the activation of peroxymonosulfate (PMS). Herein, a novel magnetic carbon-based catalyst (Fe 3 O 4 @CD-8, where 8 represents an annealing temperature of 800 ℃) with N and Fe species as catalytic active sites was fabricated to remediate sulfamethoxazole (SMX)-containing water. It showed excellent SMX removal efficiency and facilitated singlet oxygen ( 1 O 2 ) production. The characterization results revealed that Fe 3 O 4 @CD-8 had a microscopically hierarchical pore structure and an overall core–shell-like structure. Due to its large specific surface area, N-containing species, and Fe nanoparticles, 0.1 g/L Fe 3 O 4 @CD-8 removed almost 100% SMX (24 min) and achieved a 44.1% mineralization (40 min) efficiency in the presence of 0.5 mM PMS. This catalytic system also maintained its removal performance in the presence of inorganic anions and humic acids and over a wide pH range of 3–11, showing good tolerance to various environmental factors. 1 O 2 was confirmed to be the predominant active species for SMX degradation using the Fe 3 O 4 @CD-8/PMS system. Density functional theory (DFT) calculations, intermediate monitoring, and toxicity evaluation demonstrated that SMX was transformed into low-toxicity molecules and completely mineralized into CO 2 and H 2 O. The addition of Fe nanoparticles enhanced PMS adsorption and facilitated the Fe(III)/Fe(II) redox cycle to accelerate the activation of PMS. This study provides new insights and strategies for the controlled production of non-radicals for remediating antibiotic-containing wastewater.
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高影响因子
ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Yuanxiao Jin,Jiang Yu,Jie Yu,Yuerong Wu,Siwei Deng,Yinying Jiang,Zhi Huang,Donghai Wu,Weiwei Zhu
A novel carbon catalyst was created based on plant metallurgy strategy for organic pollutants removal. Plants rich in CeO 2 NPs in water were used as carbon precursors and pyrolyzed with urea to obtain Ce/N co-doped carbon catalysts, which were used in the degradation of sulfamethoxazole (SMX) by active peroxymonosulfate (PMS). The results showed that the Ce/N @BC/PMS system achieved to 94.5% degradation of SMX in 40 min at a rate constant of 0.0602 cm −1 . The activation center of PMS is widely dispersed Ce oxide nanocrystals, and CeO 2 NPs promote the formation of oxygen centered PFR with enhanced catalytic ability and longer half-life. In addition, N-doping facilitates the transfer of π-electrons within the sp2 carbon of biochar, increasing active sites and thus improving PMS activation efficiency. The degradation process was contributed to by both radical and non-radical activation mechanisms including 1 O 2 and direct electron transfer, with O 2 •- serving as 1 O 2 's precursor. Through the DFT calculations, LC-MS and toxicological analyses, the degradation pathway of pollutants and the toxicity changes throughout the entire degradation process were further revealed, indicating that the degradation of SMX could effectively reduce ecological toxicity.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ming Ma,Yuxin Lu,Sheng Wang,Shangkun Pei,Chong-Chen Wang,Xiang Li,Bo Wang
Slfamethoxazole (SMX) has been considered as one kind of important micropollutants in water which need to be removed effectively. Developing one kind of material for effectively removing SMX in water is crucial in treatment process. In this study, core–shell structured metal–organic frameworks (MOFs) with increasing shell thickness (5, 10, and 20-ZIF-8@ZIF--67 s) were selected as an ideal platform to develop water-stable hierarchical porous carbons (HPCs) using one-step calcination, showing the dual functionals of both adsorption and catalysis by producing large amount of acitve species ( 1 O 2 ). These novel HPCs systematically optimized at increasing temperatures and ratios of two metals. The 10-Co-NHPC-900 at optimal conditions shows highest adsorption capacities and initial adsorption rates, which are 4.56 and 10.35 times higher than those of calcinated ZIF-67 s. The decomposition mechanisms based on PMS were systematically studied by analyzing oxidant consumption, reactive oxygen species and by-products of SMX. In addition, Co ions leached amount of 10-Co-NHPC-900 was 63.6 times lower than that of MOF precursor, indicating that the cobalt-based porous carbon have higher water stabilities. This study offers an efficient approach for reducing micropollutants risk using water-stable hierarchical porous carbons.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jian Ke,Shangkun Zhu,Wenling Chen,Yaqin Song,Yanhua Liu,Ruixin Guo,Jianqiu Chen
The safe disposal of excess sludge has emerged as a pressing concern due to its high toxicity, stemming from a diverse array of components such as viruses, heavy metals, and polycyclic aromatic hydrocarbons. Herein, this study explored the feasibility of using extracted Fe from the excess sludge to produce metal–organic frameworks (MOFs). Specifically, MIL-100 and MIL-88A were successfully synthesized by coordinating 1,3,5-benzene tricarboxylic acid and fumaric acid with excess sludge-retained iron under wide reaction conditions. The purity of the resulting MOFs was ascertained through elemental analysis. Moreover, the synthesized MOFs demonstrated outstanding electrocatalytic performance in the degradation of sulfamethoxazole (SMX). Compared to the control group without catalysts, the addition of MIL-100-170-6 (30 mg) led to a remarkable enhancement in SMX removal efficiency, increasing it to 99.9 % from 58.3 %. This enhancement was accompanied by a substantial increase in the corresponding kinetic constant (k obs ) values, reaching 0.1137 min −1 , representing an 8.1-fold improvement over the blank group. The catalytic mechanism was further evaluated via quenching experiments and electron paramagnetic resonance (EPR) spectroscopy, suggesting that the •OH and O 2 •− radicals were responsible for SMX degradation. Economic analysis of MOF materials preparation revealed that the use of excess sludge-retained Fe can significantly reduce the cost of MOFs. Thus, it is believed that our work provides a low-cost and sustainable approach for converting excess sludge into functional MOFs, which not merely facilitates the recycling of excess sludge-retained Fe, but also provides functional materials with outstanding performance for the degradation of SMX.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shuai Yang,Dongqi Tian,Xinhao Wang,Peng Zhou,Zhaokun Xiong,Heng Zhang,Yang Liu,Gang Yao,Bo Lai
Fenton-like technology has been widely used in the field of water treatment as an advanced oxidation processes (AOPs), and a multitude of non-homogeneous catalysts have been reported effectively to enhance it. Herein, nitrogen and sulfur co-doped nanocarbon materials (NSC) was designed and synthesized, which formed a unique mesoporous structure and abundant functional groups on the surface. It exhibits superior catalytic performance to enhance the Fe(III)/H 2 O 2 system for sulfamethoxazole (SMX) degradation, k obs is 18 times higher than Fe(III)/H 2 O 2 system after the introduction of NSC under the same experimental conditions. Also, the working pH of Fe(III)/H 2 O 2 system was broadened by NSC. Quenching and probe experiments demonstrate that hydroxyl radical (∙OH) was the dominant active species. Both dissociative and surface-bound iron species were observed, which indicates direct reduction and in-situ binding of Fe(III), respectively. Further investigation found nitrogen and sulfur co-doped attribute to the formation of abundant functional groups, the C O bond and C S C bond on the surface of NSC result in the directly reduce of Fe(III), while –COOH contributes to the in-situ binding. The intermediates and possible degradation pathway of SMX degradation were proposed based on the results of liquid chromatography-quadrupole time of flight-mass spectrometer (LC-QTOF-MS). The results of cycling and co-existing ions experiments demonstrate that NSC has outstanding potential for application. This work provides a novel insight into the sustained removal of micropollutants from the aqueous environment based on the nanocarbon materials enhancing the Fenton-like oxidation.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Chuanbin Wang,Yanshan Wang,Yang Yu,Xiaoqiang Cui,Beibei Yan,Yingjin Song,Ning Li,Guanyi Chen,Shaobin Wang
The peroxymonosulfate (PMS) oxidation processes have received considerable attention for water treatment. The influence of monohydrogen phosphate and dihydrogen phosphate on PMS system is still controversial. A biochar activated PMS system was constructed to investigate the HPO 4 2− /H 2 PO 4 − effects on sulfamethoxazole degradation. Results showed that the presence of H 2 PO 4 − inhibited PMS activation, while the co-existing HPO 4 2− played a positive role. Therefore, it might be inaccurate to assess the activation capacity of a catalyst for PMS activation when using phosphate as a buffer solution. Importantly, H 2 PO 4 − inhibited the function of C O, pyridine N and defects for PMS activation. However, HPO 4 2− promoted C O and graphitic N sites for sulfamethoxazole (SMX) degradation. The contributions of OH and SO 4 − to SMX degradation decreased with the increase of H 2 PO 4 − concentration. The production of SO 4 − was accelerated with the increase of HPO 4 2− concentration, promoting pollutants degradation. The contribution of 1 O 2 first increased and then decreased with the rise of HPO 4 2− /H 2 PO 4 − concentration. This study elucidated the roles of H 2 PO 4 − and HPO 4 2− in PMS system and revealed the corresponding specific influence mechanisms, promoting the application of PMS systems for antibiotic wastewater purification.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Shizong Wang,Jianlong Wang
The surface property of biochar can be modulated through nitrogen doping and calcination temperature. In this study, nitrogen-doped sludge-derived biochar (NSDB) was prepared and applied to activate peroxymonosulfate (PMS) for sulfamethoxazole (SMX) degradation, focusing on the effect of calcination temperature on the degradation mechanism. The results showed that the contribution of free radicals to SMX degradation decreased gradually when calcination temperature increased from 300 to 800 °C. In contrast, the contribution of surface-bound reactive species increased gradually. However, the contribution of surface-bound reactive species to SMX degradation decreased for NSDB prepared at 900 °C. The change of physiochemical properties such as contact angle caused by calcination temperature was responsible for the shift of SMX degradation mechanism. NSDB prepared at 800 °C showed higher catalytic activity to PMS compared to NSDB prepared at other temperatures. Compared to sludge-derived biochar (SDB), NSDB had much higher catalytic activity, indicating that nitrogen doping could improve the catalytic activity of SDB. This study provided a way to modulate the degradation mechanism of SMX by calcination temperature of biochar to activate PMS for degradation of organic pollutants .
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
He Guo,Dongsheng Li,Zhen Li,Siying Lin,Yawen Wang,Shijia Pan,Jiangang Han
Herein, sodium percarbonate (SPC), an effective and environment-friendly oxidant, was activated by ozone (O 3 ) for promoting elimination of sulfamethoxazole (SMX) in water. The effect of various parameters including SPC dosage, O 3 dosage, SPC concentration, pH value and radical scavenger on SPC elimination was investigated firstly. Results showed that with increase of SMX dosage, the removal efficiency of SMX firstly improved and then declined. With optimal SPC dosage of 0.2 g/L, the removal efficiency of SMX rose by 16.4%, and corresponding kinetic constant multiplied by 1.7 times. Improving O 3 dosage and reducing SMX concentration were beneficial to SMX elimination. Compared with acidic and neutral conditions, alkaline condition was favorable for SMX elimination. Radical trapping experiment showed that 1 O played an important role during SMX decomposition. SPC addition could promote OH production in O 3 system. The comparison of active species in different reaction system suggested that OH and O 2 − also play crucial role for SMX elimination. TOC and COD removal were all enhanced after 30 min treatment in O 3 /SPC system. Degradation process of SMX was inspected via UV–Vis spectra, pH variation, conductivity variation and ammonia nitrogen variation. The degradation pathway was predicted by discrete Fourier transform (DFT) coupled with literatures. Finally, the toxicity of degradation intermediates was evaluated by US Environmental Protection Agency Toxicity Estimation Software Tool (US-EPA-TEST).
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高影响因子
Water
·
2025
·Vol. 17
·期 14
·2161
·
IF 3
Qiliang Xiao,Jun Nan
This study presents the development of a novel Cu–Co–O-codoped graphitic carbon nitride (g-C3N4) catalyst for efficient peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX) in aqueous environments. The synthesized Cu–Co–O-g-C3N4catalyst demonstrated exceptional catalytic performance, achieving 90% SMX removal within 10 min—significantly outperforming pristine g-C3N4(14%) and O-doped g-C3N4(22%)—with a reaction rate constant of 0.63 min−1. The superior activity was attributed to the synergistic effects of Cu-Co bimetallic doping and oxygen incorporation, which enhanced the active sites, stabilized metal ions, and minimized leaching. Mechanistic studies revealed a dual-pathway degradation process: (1) a radical pathway dominated by sulfate radicals (SO4•−) and (2) a non-radical pathway driven by singlet oxygen (1O2), with the latter identified as the dominant species through quenching experiments. The catalyst exhibited broad pH adaptability and optimal performance at neutral to alkaline conditions. Characterization techniques (XRD, FTIR, XPS) confirmed successful doping and revealed that oxygen incorporation modified the electronic structure of g-C3N4, improving charge carrier separation. This work provides a sustainable strategy for antibiotic removal, addressing key challenges in advanced oxidation processes (AOPs), and highlights the potential of multi-heteroatom-doped carbon nitride catalysts for water purification.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Chenyu Zeng,Anting Ding,Xi Chen,Yongfei Ma,Hui Lin,Han Ding,Fuyu Xie,Lu Zang,Song Cui,Ping Li,Junwei Ma,Zulin Zhang
Cu/BC-PAA (Peroxyacetic acid) system was established in this study to remove sulfamethoxazole (SMX) from waters. Cu/BC-PAA achieved high elimination efficiency (91.2 %, k = 0.081 min −1 ) for SMX within 30 min. Cu (II) loaded on corn straw biochar was converted into form Cu (I) site. Characterization, electron paramagnetic resonance (EPR), and electrochemical analysis proved that Cu (I) and C O took part in the reaction, which accelerated electron transfer and produced free radicals and non-radicals (R-O· and singlet oxygen ( 1 O 2 )). Fukui index and Liquid Chromatograph Mass Spectrometer (LC–MS) analysis revealed that sulphonamide bond cleavage and isoxazole ring opening were the main detoxification pathway. Density functional theory (DFT) calculation exhibited the adsorption energy of Cu/BC (E ads = −3.68 eV) enhanced the electron transfer between Cu (I) and PAA. The evaluation of anion effects, diverse water matrices, various sulfonamide antibiotics, and catalyst cycling tests demonstrated the Cu/BC-PAA system's exceptional stability, broad-spectrum applicability, and excellent reusability. This work successfully synthesized a stable environment-friendly catalyst for efficient activating PAA to eliminate antibiotics in waters.
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高影响因子
Journal of Water Process Engineering
·
2026
·
IF 6.6
Yize Liu,Chuanzhou Liang,Ruizhuo Lu,Zhe Liu,Xiongbo Zhan,Zhongxiong Zhou,Lin Liu,Minhua He,Bolin Li,Zhiyu Wei
Sulfamethoxazole (SMX)-degrading bacteria have been isolated previously but were rarely applied into realistic wastewater due to poor colonization and instability. In this study, an efficient SMX-degrading bacteria consortium, dominated by Pseudomonas , was enriched from activated sludge and systematically evaluated for accelerated immobilization and application in the treatment of realistic municipal wastewater. The results showed that co-substrate addition markedly enhanced consortium growth and SMX degradation. Co-substrate type further governed immobilization: glucose accelerated biofilm formation on raw carriers, whereas sucrose favored planktonic growth and required chitosan-modified electrophilic carriers for effective immobilization. Co-substrate-assisted immobilization shortened the period from over 40 d to <10 d. Moreover, the immobilized consortia exhibited a remarkably SMX degradation efficiency with ∼3 h half-life, which was strongly correlated with total attached consortium DNA ( r = 0.988). The immobilized consortia achieved stable SMX removal (>99.8%) over 30 d of cyclic operation in realistic municipal influent and effluent wastewater, respectively, proving its applicability as bio-augmentation in secondary and polishing treatment for SMX. Microbial community analysis revealed persistent Pseudomonas dominance with adaptive diversification driven by co-substrate regime, carrier type, and wastewater conditions. Overall, this study highlights rational co-substrate selection and carrier design as key determinants for efficient immobilization and long-term performance of slow-growing antibiotic-degrading consortia, providing a scalable strategy for sulfonamide antibiotics removal in wastewater treatment systems.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Qingru Chen,Ying Liu,Xiaohui Liu,Qingzhe Xu,Zheng Sun,Caili Zhang,Yongxin Li,Bin Zhao,Dawei Gao,Yan Zhang,Binbin Huang,Shenghai Huang,Maozhen Han
A novel SMX-degrading strain, Bacillus cereus SDB-X , was isolated and achieved high SMX degradation. • Strain SDB-X degrades SMX through acetylation, desulfonylation, and hydroxylamination pathways. • Adaptive mutation in the key gene menC increased enzyme–substrate binding affinity, lowering the binding energy from −8.3 to −8.6 kcal/mol. • Long-term acclimation upregulated the expression of key degradation genes, facilitating the adaptive evolution of SDB-X's SMX-degrading capability. • In complex aqueous matrices, the SDB-X strain demonstrated consistent SMX removal efficiency. Sulfamethoxazole (SMX), a widely distributed emerging contaminant, poses risks to ecosystems and public health. Microbial degradation offers an efficient and eco-friendly remediation strategy. In this study, a SMX-degrading strain was isolated from hospital wastewater and identified as Bacillus cereus SDB-X. The original strain (SDB-X00) degraded 89% of 50 mg/L SMX within five days, and after 60 days of acclimation under SMX stress, the degradation efficiency increased to 96%. Kinetic analysis revealed that the acclimated strain SDB-X60 exhibited the fastest degradation rate ( k = 0.721 d −1 , t ₁/₂ = 0.96 d). Moreover, SDB-X60 maintained stable degradation activity in a complex wastewater matrix. LC-MS/MS analysis proposed a tentative SMX metabolic pathway involving N -acetylation and typical intermediate metabolites. Genomic analysis identified several candidate degradation-related genes; a mutation in SDB-X60 altered the MenC protein substrate binding free energy from −8.3 to −8.6 kcal/mol. Transcriptomic analysis further indicated upregulation of degradation-related genes after acclimation. This study expands understanding of SMX biodegradation by B. cereus and highlights the role of acclimation in enhancing degradation activity, providing a theoretical basis for bioremediation of antibiotic-contaminated environments.
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高影响因子
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