Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Adeel Ahmed,Muhammad Usman,Zhijian Ji,Muhammad Rafiq,Raza Ullah,Bing Yu,Youqing Shen,Hailin Cong
In this work, an environmentally friendly reduced graphene oxidized supported cobalt ferrite (CFO/rGO) catalyst was constructed using a hydrothermal technique to heterogeneously activate peroxymonosulfate (PMS) and utilized for the degradation of sulfamethoxazole (SMX) antibiotic in aqueous solution. The results exhibited that the complete degradation of SMX was achieved in 25 min under optimal conditions ([SMX] = 8.0 mg/L, [CFO/rGO-30%] = 0.5 g/L, [PMS] = 5.0 mM, pH = 7.0) in the presence of CFO/rGO-30%/PMS with a rate constant of 0.3076 min ˗1 , which was roughly 6.08 times higher compared to the CoFe 2 O 4 /PMS system (0.0506 min ˗1 ). The enhanced degradation of SMX in the CFO/rGO-30%/PMS system might be attributed to the large surface area of the CFO/rGO-30% (98.11 m 2 /g) catalyst compared to the pristine CoFe 2 O 4 (24.31 m 2 /g), which increased the availability of active sites for PMS activation . Furthermore, the influence of pivotal reaction parameters and interfering anions on SMX mineralization was also scrutinized. The formation of free radicals (SO 4 •− , • OH, and 1 O 2 ) was established through quenching experiments and electron paramagnetic resonance analysis. The degradation mechanism of SMX was speculated based on the identification of degradation intermediates and X-ray photoelectron spectroscopy spectral analysis. Mechanistic investigations suggested that the transition of Co 2+ /Co 3+ and Fe 3+ /Fe 2+ pairs on the catalyst surface was responsible for the PMS activation, and the SMX degradation was accomplished through radical and non-radical pathways. Furthermore, CFO/rGO-30% exhibited high stability after four consecutive cycles and maintained catalytic activity . Finally, the developed CFO/rGO-30% catalyst exhibited promising potential for the purification of SMX polluted water.
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Frontiers in Chemistry
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2025
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IF 4.2
Xianbing Zhang,Yuheng Liu,Jiajia Yuan
Metal-organic frameworks (MOFs) are recognized as important Fenton-like materials for environmental remediation. However, their applications are often hindered by slow cycling between Fe (III) and Fe (II). This study aimed to address the slow Fe (III)/Fe (II) cycling limitation of Fe-MOFs through dual modification strategy: bimetallic modification and amino functionalization. A series of NH2-MOF(Fe, Co) catalysts with varying Fe/Co ratios were synthesized via a hydrothermal method and evaluated for sulfamethoxazole (SMX) degradation. The optimized NH2-MOF(Fe, Co) catalyst (Fe/Co ratio = 7:3) exhibited substantially enhanced catalytic performance, with SMX removal rate and rate constant in the H2O2 system being 3.2 and 43.5 times higher than those of the Fe-MOF/H2O2 system, respectively. The catalyst demonstrated robust performance across a wide pH range (3.05–7.00), addressing a common limitation of Fenton-like systems. Physicochemical characterization revealed that the enhanced performance was attributed to two key factors: the synergistic effect between Co and Fe in the bimetallic active center, and improved electron transfer to the central metal due to -NH2 functionalization. These modifications effectively addressed the Fe (III)/Fe (II) redox cycling limitation. The proposed reaction mechanism provides insights into SMX degradation pathways in the NH2-MOF(Fe, Co)/H2O2 system. This study presents an efficient and stable MOF-based Fenton-like catalyst with potential applications in wastewater treatment and environmental remediation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Feitong Chen,Yulin Fan,Zhuohan Lin,Zhixian Li,Xueqing Qiu,Hongming Lou,Yuxia Pang
This study presents a pH-switchable Fenton-like system based on sulfur-doped FeP synthesized via a confined gas–solid strategy, where ·OH dominates at pH 3.0 and Fe(IV)=O prevails at pH 6.0. Sulfur incorporation modulates the FeP electronic structure by expanding the lattice, enhancing Fe–P covalency, and increasing electron density, thereby promoting charge transfer and reducing the activation barrier for H 2 O 2 activation. The optimized FePS 15 catalyst achieved ~99% sulfamethoxazole degradation (150 mg/L) within 15 minutes, exhibiting a reaction rate 2.54 times higher than that of undoped FeP. When further supported on lignin-derived carbon spheres (FePS 15 @LC), it exhibited enhanced structural integrity, suppressed iron leaching, and improved reusability. These findings demonstrate that sulfur doping drives pH-dependent ROS switching from ·OH to Fe(IV)=O, supporting adaptable Fenton-like catalysis. This work improves mechanistic insight into ROS modulation and enables pH-adaptable advanced oxidation processes for pollutant removal.
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BIORESOURCE TECHNOLOGY
·
2025
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IF 9
Yu Zhang,Yajing Liu,Yelei Li,Hu Cheng,Changyin Zhu,Yu Shen,Sicheng Shao,Jianming Xue,Dongmei Zhou,Fuliang Cao
The low-cost transformation of agricultural biowaste into high-value biochar materials presents substantial technological and economic challenges. In this study, we report for the first time that soda residue can effectively substitute for chemical activation agents to produce micro/mesoporous biochars (MMBs) with a well-developed specific surface area (473.73 m 2 g −1 ) and pore volume (0.55 cm 3 g −1 ). These MMBs exhibit exceptional sorption capacity for the antibiotic sulfamethoxazole in aqueous solutions, reaching a maximum sorption capacity of 92.97 mg g −1 . The sorption mechanism is governed by multiple interactions, including pore filling, hydrogen bonding, partitioning, electrostatic interactions, and π-π stacking. MMBs demonstrate superior stability, excellent reusability, cost-effectiveness, environmental compatibility, and strong anti-interference capability, rendering them highly suitable for practical applications. This study opens new avenues for the sustainable recycling of soda residue and biowaste and the fabrication of high-performance porous biochars while also providing an efficient and eco-friendly sorbent for environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Mingze Sun,Shaojuan Yan,Hang Gao,Hongxuan Chu,Wanying Tong,Donglin Zhao,Hongwen Yu,Jianhua Qu,Ying Zhang
Effectively scavenging combined pollutants in complex water matrix via dominant electron transfer pathway using modified zero-valent iron (ZVI) remains challenging. Herein, novel iron-based catalysts were synthesized using ball milling and pre-oxidation modified biochar (MOBC), which featured abundant pore structure and oxygen-rich functional moieties to support nZVI in activating persulfate (PS). The most suitable catalytic system achieved ultrafast simultaneous removal of 89.0 % of sulfamethoxazole (SMX) and nearly 100 % of hexavalent chromium (Cr(VI)) within 5 min (with nearly complete removal of SMZ and Cr(VI) in 60 min). By serving as an electron shuttle, MOBC 700 could accelerate electron transfer from SMX to PS adsorbed on the nZVI 1.0 @MOBC 700 for SMX decomposition, with reactive oxygen species (ROSs) also contributing. Moreover, nZVI facilitated the reduction of Cr(VI) adsorbed on nZVI 1.0 @MOBC 700 through electron transfer. The dissolved Fe(II) generated via PS activation and Cr(VI) reduction further facilitated Cr(VI) removal from the solution, while the gradual consumption of excess Fe(II) ensured continued ROSs-mediated degradation of SMX. Additionally, the system also demonstrated resistance to interference from NO 3 - , CO 3 2- , and humic acid, and was effective in remediating four different water samples. Overall, this study presents a promising method for designing iron-char composites to address combined antibiotic and heavy metal contamination in groundwater samples via dominant electron transfer process.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jian Wei,Zhaokun Xiong,Mengmeng Ao,Zhuang Guo,Jiali Zhang,Bo Lai,Yonghui Song
Fe-based catalysts activating peroxymonosulfate (PMS) for the generation of hydroxyl radicals ( OH) and sulfate radicals (SO 4 − ) have attracted widespread interest to efficient degrade contaminants. However, their limitations, including the leaching of metals and the instability of free radicals, are still thorny issues that plague researchers. In this study, an N-doped graphite catalyst (Fe-NC-4) was developed to activate PMS for the degradation of sulfamethoxazole (SMX). Transmission electron microscopy, X-ray diffraction and Raman spectroscopy found that Fe N active site was evenly distributed in the catalyst, and the iron leached under any experimental conditions was far below the instrument detection limit. Fe-NC-4 performed superior capacity in PMS activation, as evidenced by approximately 100% degradation of SMX after 10 min of treatment. Multiple experiments confirmed that OH, SO 4 − , and superoxide radical (O 2 − ) exerted negligible contribution. The Fe-NC-4/PMS system degraded SMX mainly through non-radical pathway of singlet radical ( 1 O 2 ) and high-valent iron-oxo species ( Fe(Ⅳ) O). Moreover, the Fe-NC-4/PMS system had satisfactory stability in natural water and showed excellent selective oxidation of different contaminants. This work will shed new light on effective PMS activation by Fe-based catalysts to efficiently degrade aqueous contaminants via the non-radical pathway.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
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IF 7.8
Weitao Kong,Zhongmou Liu,Jinghui Wu,Chenying Wen,Juncheng Yan,Yidi Gao,Guanqiao Li,Xianze Wang,Mingxin Huo
This study investigates the degradation of sulfamethoxazole (SMX), a widely detected and persistent antibiotic in the environment, using a novel photocatalytic system based on MIL-101(Fe) supported Mo single-atom with oxygen vacancies (Mo/Ov-MOF). Anchoring Mo single-atoms into the MOF structure enhances catalytic activity by effectively improving charge separation and reducing electron-hole recombination. The Mo/Ov-MOF efficiently activates peroxymonosulfate (PMS) under visible light, generating singlet oxygen ( 1 O 2 ) as a primary reactive species responsible for SMX degradation. Degradation experiments demonstrated that the degradation efficiency reached 96.8 % in the presence of PMS and visible light. Through quenching and trapping experiments on active species, an in-depth investigation into the source of 1 O 2 was performed, demonstrating the crucial role of holes in the rapid and selective generation of 1 O 2 under visible light. Additionally, the reusability of the Mo/Ov-MOF catalyst was confirmed, maintaining over 70 % degradation efficiency after five cycles. Toxicity assessments indicated that the degradation by-products exhibited significantly lower toxicity than the parent compound SMX, thus mitigating potential ecological risks. The mechanistic insights reveal that oxygen vacancies and Mo single-atom enhance electron transport and facilitate efficient PMS activation, ultimately leading to effective pollutant degradation. The findings underscore the potential of the Mo/Ov-MOF photocatalytic system for practical applications in wastewater treatment, particularly for removing persistent organic pollutants from aquatic environments.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jiajun Zou,Yanjun Shao,Xinyu Hu,Haichuan Zhang,Shanshan Ye,Ji Li
Sieving effect of pores was key of mitigating the natural organic matters (NOMs) interference to selectively remove antibiotics from wastewater. Yet the pore structures of porous materials were varied and complicated, bringing huge difficulty for exploring the relationship between pore structure and sieving effect. To address this, three typical MCs were accurately synthesized to own the interconnected hierarchically-spherical pore ( ic -HSMC), interconnected ordered slit-like pore ( ic -SMC) and isolated ordered tubular pore ( is -TMC). Under the weak interference of humic acid, smaller uniform mesopore size has a stronger size-exclusion effect to sieve sulfamethoxazole (SMX) and large-molecular humic acid (HA), resulting in higher capacity retention rates (CRR) of >91% for ic -SMC (4.2 nm) and is -TMC (3.5 nm) than 84.4% for ic -HSMC (2.7–74.4 nm). With HA concentration increasing (15 mg·L −1 ), because more transport channels effectively mitigate the pore-blocking effect of HA, ic -HSMC and ic -SMC with interconnected pores showed a close CRR of ∼54% (only 44.6% of is -TMC with isolated pores). Notably, when HA concentration was much large to 30 mg·L −1 , the highest CRR of ic -HSMC still maintained at 50.9% (30.9% of is -TMC and 39.3% of ic -SMC), resulting from more external surface (45% S BET ) of hierarchically-spherical macropores to disperse HA and disordered channels to resist HA transport into internal adsorption sites. Above all, the internal pore structure of MCs (connectivity, shape and order degree) played a crucial role in mitigating the interference of NOM, providing a new perspective on porous adsorbents/catalysts design for highly-selective antibiotics removal from wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Mingjun Li,Jifeng Zhao,Xin Zhao,Peihao Yan,Shiyuan Wei,Zizhang Guo,Jian Zhang,Huijun Xie,Haiming Wu
MFCMEcw achieved the highest sulfamethoxazole removal efficiency (69.66%) • Bioelectrochemistry alleviates greenhouse gas emissions under SMX stress • Bioelectrochemistry enriched electroactive bacteria • MFCMEcw increased the risk of resistance gene transmission Sulfamethoxazole (SMX) is widely detected in natural aquatic environments and poses increasing environmental concerns due to its persistence and incomplete removal in conventional treatment systems. Therefore, developing green and sustainable treatment technologies to remove SMX remains a critical challenge. In this study, the bioelectrochemical technologies including microbial fuel cell-integrated (MFCMEcw) and externally powered electrolysis cell (ECMEcw) were integrated with iron‑carbon micro-electrolysis constructed wetlands (MEcw) to evaluate their long-term (240 days) treatment performance, microbial responses, and ecological risks under SMX exposure. MEcw exhibited the highest removal efficiencies of total nitrogen (29.51%) and total phosphorus (57.77%), indicating greater resistance to antibiotic stress. In contrast, MFCMEcw achieved the highest SMX removal efficiency (69.63%), accompanied by significant reductions in greenhouse gas emissions and global warming potential. Metagenomic analysis revealed that MFCMEcw enriched electroactive microorganisms and extracellular electron transfer-related genes, suggesting increased electron transfer-related functional potential. However, antibiotic resistance genes, mobile genetic elements, and virulence factors were simultaneously enriched, indicating elevated ecological risks associated with resistance dissemination. Multivariate analyses further suggested that bioelectrochemical regulation, iron-associated processes, and microbial functional potential were closely associated with pollutant attenuation and environmental responses in the CWs. These findings provide insights for optimizing sustainable treatment technologies for antibiotic-contaminated wastewater. Download: Download high-res image (204KB) Download: Download full-size image
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 5
·1-12
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IF 6.408
Hu Wenyao,Chen Yanlong,Xia Ling,Hu Yufei,Li Gongke
A sepiolite/chitosan/silver nanoparticles (Sep/CTs/AgNPs) membrane substrate has been developed for the fast separation, enrichment, and surface-enhanced Raman scattering (SERS) determination of sulfamethoxazole all-in-one. The Sep/CTs/AgNPs membrane substrate possessed the ability of rapid separation and enrichment to simplify the process for pretreatment and improve the efficiency of analysis. The grown AgNPs can provide abundant hot spots and plasmonic areas to amplify the Raman signals of target molecules effectively. The membrane substrate exhibited good stability with relative standard deviations of 5.8% and 7.1% to same batch and different batches membrane substrate, respectively, by detecting sulfamethoxazole. The SERS method based on Sep/CTs/AgNPs membrane substrate was used for the determination of sulfamethoxazole with a linear range of 0.05–2.0 mg/L, and the limit of detection was 0.020 mg/L. The established SERS method was finally applied to the quantification of sulfamethoxazole in animal-derived food samples. Sulfamethoxazole was actually found in crucian sample with 12.4 μg/kg, and the result was confirmed by a high-performance liquid chromatography method with relative error of 5.3%. The whole process of analysis can be finished within 25 min with recoveries of 89.3–102.2%. The SERS method based on Sep/CTs/AgNPs membrane substrate provided an integrated strategy for rapid and accurate SERS analysis in food safety issues. Graphical abstract
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Analytical Methods
·
2021
·Vol. 13
·期 42
·5075-5084
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IF 2.896
Lu-Zhu Chen,Hai-Long Wu,Wan-Jun Long,Tong Wang,Gao-Yan Tong,Ru-Qin Yu
In this work, a simple and fast analytical method based on a self-weighted alternating trilinear decomposition (SWATLD) algorithm coupled with excitation–emission matrix (EEM) fluorescence was developed for the simultaneous determination of sulfamethoxazole (SMZ) and trimethoprim (TMP) illegally added to health products. With the second-order advantage, the proposed method obtained satisfactory results in the presence of peak overlap and unknown interferences. The analysis time for a single sample is only 0.8 minutes. The average spiked recoveries of SMZ and TMP in three health product spiked samples were in the range of 91.0–106.2% and 86.8–107.8%, respectively. The relative standard deviations (RSDs) were lower than 8.6%. In addition, verification parameters including sensitivity (SEN), selectivity (SEL), the limit of detection (LOD), the limit of quantification (LOQ), intra-day precision, and inter-day precision were calculated, and the results show that the proposed method is feasible. The quantitative results of the proposed method were further confirmed by the LC-MS/MS method, which proved that the proposed method was efficient and green for drug-abuse monitoring of SMZ and TMP in health products.
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ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Shengnan Li,Xuya Zhu,Hang Yu,Xizi Wang,Xiaqing Liu,Hui Yang,Fengxiang Li,Qixing Zhou
Antibiotic wastewater presents serious challenges in water treatment . Metal-organic frameworks (MOFs) have received significant attention as promising precursors and sacrificial templates in the preparation of porous carbon-supported catalysts. Herein, we investigated the sulfamethoxazole (SMX) degradation and electrochemical performance of microbial fuel cells (MFCs) that applied as-prepared Ni-MOF-74 and Ni–N–C (Ni-MOF-74 underwent pyrolysis treatment at different temperatures) as air-cathode catalyst. Firstly, the electrocatalytic activity towards oxygen reduction reaction (ORR) of the catalyst was investigated by rotating disk electrode. The results showed that electron transfer number for Ni-MOF-74 was 2.12, while that of 800Ni–N–C was 3.44, which was close to four-electron reduction. Applying Ni-MOF-74 in MFCs, a maximum power density of 446 mW/m 2 was obtained, which was close to that of 800Ni–N–C. Besides, using Ni-MOF-74 as cathode catalyst, a chemical oxygen demand removal rate of about 84% was obtained, and the degradation rate of 10 mg/L SMX was 61%. The degradation rate decreased with increasing antibiotic concentration, but the average degradation efficiency increased stepwise. Additionally, the relative abundance of resistant gene sul1 in the reactors of the new catalytic material was about 62% lower than that of sul1 in the control (Pt/C) reactors, and the relative abundance of sul2 was about 73% lower. Moreover, cost assessments related to the catalyst performance are presented. The findings of this study demonstrated that Ni-MOF-74 could be considered as a two-electron transfer ORR catalyst, and offers a promising technique for preparation of Ni–N–C for use as four-electron transfer ORR catalysts. In comparison, Ni-MOF-74 could be a promising ORR catalyst of MFCs for antibiotic degradation.
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