CHEMICAL PAPERS
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2026
·
IF 2.7
Hu Zhijun,Zhang Juntao,Wei Benmei,Li Sheng,Long Yangke
Porous carbon derived from waste biomass exhibits significant potential for removing environmental contaminants due to its adsorptive properties. However, a structural trade-off exists between achieving the high porosity necessary for optimal adsorption capacity and the high energy consumption with equipment corrosion resulting from the pore-forming process. In this study, a novel strategy based on a free-radical-assisted hydrothermal process was presented for synthesizing porous biochar. Peroxymonosulfate (PMS) serves as the free radical source, enabling controlled oxidation of corn stalk pith during a straightforward hydrothermal pretreatment at 120 °C, followed by carbonization at 700 °C to form internal pores. This innovative approach enhanced the sulfamethoxazole (SMX) adsorption capacity by approximately threefold, from 43.37 mg/g to 130.22 mg/g. Although the PMS-pretreated porous biochar surface displayed superhydrophilic properties due to carboxyl group modification, results analyses indicate that SMX adsorption is primarily driven by π–π conjugation, hydrophobic interactions, and hydrogen bonding, relying on specific surface area rather than electrostatic interactions. This study presents a beneficial attempt at a free-radical-based pretreatment for the straightforward and robust synthesis of porous biochar. Graphical abstract The alternative text for this image may have been generated using AI.
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Toxics
·
2026
·Vol. 14
·期 6
·457
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IF 4.9
Xu Ding,Xin Li,Haojie Liu,Zhong Li,Yangchun Xia,Yanpeng Liang,Honghu Zeng,Xiaohong Song
Ofloxacin (OFL) and sulfamethoxazole (SMX) are common co-occurring antibiotic contaminants in aquatic environments, yet their long-term combined toxicity to freshwater fish remains poorly elucidated. In this study, adult mosquitofish (Gambusia affinis) were used as a model to investigate histopathological alterations, oxidative stress responses, gene expression, and gut microbiota changes after 30 days of exposure to environmentally relevant concentrations of OFL and SMX (0 ng/L, 50 ng/L, 1 μg/L, and 20 μg/L), either individually or in combination. The results showed that both single and combined exposures induced liver and intestinal damage. Oxidative stress responses exhibited clear tissue specificity, with activation of antioxidant defenses in the liver, whereas the intestine was mainly characterized by decreased SOD and GST activities, as well as reduced MDA content. Changes in gene expression were relatively limited, with significant alterations observed only in hepaticsod2andhsp90and intestinalhsp70in certain treatment groups. Gut microbiota analysis showed that OFL exerted a stronger disruptive effect than SMX, as reflected by increased alpha diversity, reduced abundance of core genera, and functional remodeling, whereas combined exposure triggered weaker microbial community restructuring relative to single exposures. Overall, OFL and SMX induced tissue-specific toxicity in mosquitofish by causing tissue injury, oxidative stress imbalance, and gut microbiota dysbiosis, with OFL showing the stronger overall effect.
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CHEMICAL ENGINEERING JOURNAL
·
2026
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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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DESALINATION
·
2026
·
IF 9.9
Yuxuan Zhu,Haikuo Lei,Zengli Dai,Dong Liang,Quan Kang,Hongqing Lv,Huichao Su
A cathodic EMR equipped with highly dispersed Co/Fe-doped CoFeCM achieves 99.4% removal of high-concentration SMX. • FeCoN 6 -like local sites synergistically generate ·OH and O 2 · − for efficient removal. • Chitosan enhances metal anchoring and membrane flexibility, enabling low-cost fabrication. • Continuous-flow EMR realizes electrocatalytic oxidation and membrane separation in one single unit. To address the low efficiency and poor environmental safety of traditional technologies for degrading sulfamethoxazole (SMX), a cathodic electrocatalytic membrane reactor (EMR) was constructed by integrating CoFeCM as the cathode. CoFeCM was fabricated via a scalable mechanical ball milling-hot pressing‑carbonization route using chitosan-modified activated carbon as the substrate, where chitosan enhanced the anchoring of highly dispersed Co/Fe sites to suppress agglomeration and improved membrane mechanical flexibility. The equimolar Co₅Fe₅CM exhibited optimized porous structure (BET: 541.3 m 2 /g), excellent electrical conductivity (8542 S/m), and superior oxygen reduction reaction (ORR) activity. Under mild conditions (1.2 V, pH 3), the EMR achieved 99.4% removal of 100 mg/L SMX and 45.3% COD removal, with 12.4% TOC removal indicating effective transformation and partial mineralization. Mechanistic investigations confirmed that Fe Co sites formed a FeCoN 6 -like local structure with site-specific synergy. Fe sites thermodynamically favored 2e − ORR for efficient H 2 O 2 production, while Co sites kinetically promoted 1e − activation of H 2 O 2 to ·OH. ·OH and O 2 · − served as dominant active species, enabling multi-pathway SMX removal through sulfonamide bond cleavage and oxazole ring opening, with significantly reduced biotoxicity of intermediates. The EMR maintained stable removal efficiency (93.1% after 10-day continuous operation), and the concentrations of Co and Fe in the effluent were lower than the instrumental detection limit, and exhibited good universality for various refractory pollutants, providing a green, cost-effective, and scalable solution for antibiotic-contaminated wastewater treatment, and further demonstrates great potential for simultaneous organic pollutant elimination and salt rejection in high-salinity desalination wastewater systems, broadening the application boundary of electrocatalytic carbon membranes for seawater desalination and brine resource utilization. Download: Download high-res image (128KB) Download: Download full-size image
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ACS ES&T Water
·
2025
·
IF 4.3
Chunhui Zhang,Jing Ji,Huijie Hu,Fuyu Li,Ruomeng Li,Peng Zhang,Cuiping Wang,Hongwen Sun
Biochar (BC) is widely used in persulfate (PS)-based advanced oxidation processes (AOPs), yet the environmental role of biochar-derived dissolved organic matter (BDOM) remains poorly understood. Here, we revealed that BDOM released from BC pyrolyzed at 300–700 °C regulated the oxidation degradation of sulfamethoxazole (SMX) in a ball-milled N-doped BC-ZVI (NBC-ZVIbm)/PS system. Results showed that higher pyrolysis temperatures produced a lower-molecular-weight BDOM with more oxidized species. Although pyridinic and graphitic N in NBC-ZVIbm enhanced PS activation and electron transfer, BDOM significantly suppressed SMX degradation, with stronger inhibition observed at higher pyrolysis temperatures. Quenching experiments combined with Fourier infrared cyclotron resonance mass spectrometry (FT-ICR-MS) analyses identified aliphatic polyphenols and lignans as the dominant inhibitory components. Key molecular features including O/C and H/C ratios and the abundance of −OH groups and unsaturated bonds were strongly correlated with reduced SMX removal. Further mechanistic analysis revealed that BDOM hindered degradation through multiple pathways: consuming oxidants, scavenging reactive species, chelating iron ions, and altering transformation routes. This work highlights the underappreciated inhibitory role of BDOM and suggests the avoidance of excessive pyrolysis temperatures to improve the practical efficacy of BC-mediated AOPs for environmental remediation.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2023
·
IF 6
Shupeng Lin,Ziqi Shen,Deng Pan,Rongting Ji,Yongrong Bian,Jiangang Han,Xin Jiang,Yang Song,Hu Cheng,Jianming Xue
Marine macroalgae are promising biomass resources due to their fast growth, high yield and special composition and urgently need to be developed. Pyrolytic conversion of marine macroalgae into stable and multifunctional biochars is an extremely feasible strategy, but there are few related studies, especially on further decontamination applications and performance. In this study, the green tide-derived marine macroalga Enteromorpha prolifera was used to prepare multielement-doped porous biochars (MPBs) and applied to remove a typical antibiotic, sulfamethoxazole (SMX), from aqueous solution for the first time. The MPBs possess a porous structure, and the specific surface area and pore volume are as high as 134 m 2 g −1 and 0.030 cm 3 g −1 , respectively. The surface N, O, S and Cl contents of the MPBs are high. An abundant ash content, O-containing surface functional groups and graphene structure also exist in the MPBs. These excellent properties contribute to a high sorption quantity, up to 30 mg g −1 . Pore filling, n/π-π stacking, cation bridging interactions, electrostatic attraction, hydrogen bonding and partitioning are the potential sorption mechanisms. Moreover, the sorption is controlled by physical processes; monolayer sorption is relevant for low carbonization temperature-derived MPBs, and multilayer sorption is relevant for high carbonization temperature-derived MPBs. In addition, the removal capacity of SMX changed slightly after 4 cycles. The findings suggest that marine macroalgae can be deemed excellent precursors for the preparation of MPBs-based sorbents for organic pollutants.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·71088-71102
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IF 5.8
Fan Xinfei,Liu Na,Yang Jia,Yu Yueling,Xu Yuanlu,Song Chengwen,Liu Yanming
Persulfate activation is emerged as an alternative applied in environment remediation, but it is still a great challenge to develop highly active catalysts for efficient degradation of organic pollutants. Herein, a heterogeneous iron-based catalyst with dual-active sites was synthesized by embedding Fe nanoparticles (FeNPs) onto the nitrogen-doped carbon, which was used to activate peroxymonosulfate (PMS) for antibiotics decomposition. The systematic investigation indicated the optimal catalyst exhibited a significant and stable degradation efficiency of sulfamethoxazole (SMX), in which the SMX can be completely removed in 30 min even after 5 cycle tests. Such satisfactory performance was mainly attributed to the successful construction of electron-deficient C centers and electron-rich Fe centers via the short C-Fe bonds. These short C-Fe bonds accelerated electrons to shuttle from SMX molecules to electron-rich Fe centers with a low transmission resistance and short transmission distance, enabling Fe (III) to receive electrons to promote the regeneration of Fe (II) for durable and efficient PMS activation during SMX degradation. Meanwhile, the N-doped defects in the carbon also provided reactive bridges that accelerated the electron transfer between FeNPs and PMS, ensuring the synergistic effects toward Fe (II)/Fe (III) cycle to some extent. The quenching tests and electron paramagnetic resonance (EPR) indicated O 2 ·− and 1 O 2 were the dominant active species during the SMX decomposition. As a result, this work provides an innovative method to construct a high-performance catalyst to active sulfate for organic contaminant degradation.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Weichen Zeng,Han Zhang,Rui Wu,Luming Liu,Guibai Li,Heng Liang
This study focused on the preparation, characterization, and sulfamethoxazole (SMX) removal performance of the SnO 2 -coated reactive electrochemical membrane (REM). This REM was fabricated by loading SnO 2 on the reduced TiO 2 nanotube arrays (RTNA)-based Ti membrane (TM). Regarding the dopant for SnO 2 , Sb was more effective in boosting the electrocatalytic activity than Bi, and the energy consumption for Sb-SnO 2 -coated REM (TM/RTNA/ATO) was lower than Bi-SnO 2 -coated REM (TM/RTNA/BTO). As for the internal layer, RTNA provided TM/RTNA/ATO with more electroactive surface areas and prolonged the service lifetime. Compared with batch mode, the SMX removal efficiency in flow-through mode was increased up to 8.4-fold. The SMX degradation performances were also affected by fluid velocity, current density, initial SMX concentration, and electrolyte concentration. The synergistic effects of • OH oxidation and direct electron transfer were responsible for the effective removal of SMX. TM/RTNA/ATO was proved to be stable and durable by multi-cycle and accelerated lifetime tests. Its extensive applicability was verified with high removal efficiencies of SMX in the surface water and wastewater effluent. These results demonstrate the promise of TM/RTNA/ATO for water treatment applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Lei Zhou,Yubo Yan,Hengyang Mao,Shouyong Zhou,Jiayu Hui,Haodong Li,Meisheng Li,Yijiang Zhao,Qi Zhang,Shanshan Xia
Antibiotic contamination of aquatic ecosystems has attracted growing concern over the past few years. As a novel and low-cost catalytic membrane, attapulgite-based ceramic membrane (ATPCM) impregnated with Co 3 O 4 (Co-ATPCM) was successfully prepared for the degradation of sulfamethoxazole (SMX) under peroxymonosulfate (PMS) activation. The physical and chemical properties of ATPCM and Co-ATPCM were characterized by SEM-EDS, XRD, XPS, zeta potential, contact angle and the three-point bending test. Co was stably anchored on ATPCM via X-O-Co (X denotes Al, Si or Mg) bonds during the catalytic process, avoiding Co leaching. Approximately 70 % SMX could be removed by the optimized Co-ATPCM in batch experiments over a wide pH range from 4.0 to 10.0. Furthermore, 58 % SMX degradation was observed during filtration experiments with a high water flux of up to 774 L m −2 h −1 (LMH). According to the quenching experiment and electron paramagnetic resonance (EPR) spectroscopy, SO 4 − , OH and 1 O 2 were involved in the SMX degradation process, while 1 O 2 played a dominant role. Density functional theory (DFT) calculation successfully predicted that the sits on SMX molecules with high Fukui index were more susceptible to attacks by free radicals, confirmed by liquid chromatography-Quadrupole-time of flight mass spectrometer (LC-MS). Consequently, a possible pathway for the catalytic oxidation process was proposed based on the results of DFT and LC-MS. This study provided a promising strategy using natural magnesium aluminum silicate clay minerals to prepare cost-effective, efficient, and eco-friendly catalytic membranes for wastewater treatment.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Jinlong Zhang,Wenjing Yang,Xingyu Liu,Fan Su,Gang Wang,Sihui Zhan,Yi Li
Although the electro-Fenton (EF) process is effective for wastewater treatment , recycling spent catalysts remain a major challenge. Therefore, we introduce a reuse strategy for spent catalysts where an iron hydroxyphosphate [Fe 5 (PO 4 ) 4 (OH) 3 ·2H 2 O] catalyst is utilized. Fe 5 (PO 4 ) 4 (OH) 3 ·2H 2 O obtained •OH and •O 2 − by activating in-situ produced H 2 O 2 , and the degradation rate of sulfamethoxazole reached 94.5% after 120 min and showed excellent stability (maintained above 90%) for 10 cycles. Finally, the used catalyst was converted into slow-release ammonium ferrous phosphate (NH 4 FePO 4 ·H 2 O) fertiliser at a conversion rate of 85.6%. NH 4 FePO 4 ·H 2 O significantly promoted plant and seed growth within 6 days, highlighting the contribution of the resource recycling of the spent catalyst. This study serves as a valuable reference for the efficient utilization of spent catalysts. This study successfully applied EF catalysts and explored the recycling of spent catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yue Zhao,Rui Gao,He Wang,Yanping Sun,Xiaohui Zhan,Lei Chen,Junyan Liu,Huixiang Shi
The adsorption and protective calcination methods were combined to synthesize single Mn atoms catalyst with more Mn-N x exposure for peroxymonosulfate (PMS) activation. During the carbonization process, the surface adsorbed Mn species in zeolitic imidazolate framework-8 (ZIF-8) and the surrounding graphitic carbon nitride (g-C 3 N 4 ) jointly maintained the morphology of precursor and enriched Mn-N 6 sites near the catalyst surface. The hollow and hierarchically porous structures induced by the erosive function of g-C 3 N 4 further facilitated the exposure of Mn-N 6 sites and mass transfer processes. Herein, the derived hollow carbon polyhedron catalyst (C-Z8-Mn@g-C 3 N 4 ) possessed highly accessible edge-host Mn-N 6 sites and ultra-high specific surface area (1846.91 m 2 g −1 ). C-Z8-Mn@g-C 3 N 4 exhibited remarkable catalysis for sulfamethoxazole (SMX) degradation at an extremely low dosage (0.01 g L −1 ), particularly, up to 3.8 times of promotion was obtained compared to traditional single Mn atoms catalyst (66.9 vs 17.8 L g −1 min −1 ). Besides, the catalytic performance of C-Z8-Mn@g-C 3 N 4 was not obviously affected by initial pH (3.14–11.00), inorganic anions and natural organic matters (NOMs). Experiments and Density functional theory (DFT) calculations revealed that Mn-N 6 sites not only had stronger PMS adsorption capacity than graphitic N, but also enhanced the electron transfer between catalyst and PMS, thus promoting the redox and self-decomposition of PMS to produce SO 4 − , OH and singlet oxygen ( 1 O 2 ) (as major active oxygen species). This work provides new insights into the regulation of active sites exposure in single-atom catalysts for enhanced catalytic performance.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wenjie Wu,Liang Bai,Yenan Song,Yuanting Su,Kai Jiang,Haitao Sun,Guangyin Zhen,Yan Shen,Qinghong Yuan,Zhuo Sun
Graphene-based catalysts have been widely applied for catalytic ozonation. However, as it is difficult to obtain graphene with high structural precision, it is currently unfeasible to comprehend the relationships between the intrinsic structure of the layered carbon catalysts with its catalytic activities. Here, an advanced plasma-assisted etch strategy was used to fine tune the ozonation activity of monolayered graphene films by tailoring the defect types. Raman mapping indicated that the defects of the as-prepared monolayered graphene films were predominantly sp3, vacancy, and boundary-type defects, respectively. The roles and contributions of these active defects in manipulating the oxidative potential of monolayered graphene films were revealed by quenching experiments, electron paramagnetic resonance results, and density functional theory calculations. The catalytic results showed that the monolayered graphene films with boundary-like defects exhibited the best catalytic performance toward the degradation of sulfamethoxazole. This work contributes new insights into the design of high-efficiency carbonaceous catalysts by structuring additional defective sites.
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