JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Xinyuan Wang,Zhuohang Wu,Taozhen Li,Xiaoning Wang,Pijun Duan,Jingwen Pan,Lei Wang
Sulfonamide antibiotics are highly toxic, persistent, and environmentally hazardous, necessitating effective remediation technologies for their removal from aquatic systems. Singlet oxygen ( 1 O 2 ), a selective and pH-tolerant reactive species, has emerged as a key oxidant in persulfate-based advanced oxidation processes (PS-AOPs). Herein, the systematic and novel pathway formation for the 1 O 2 on single Cu atom during PS-AOPs was elucidated. Nitrogen-doped biochar-supported single-atom Cu catalysts featuring low-coordination Cu-N 2 sites (SACu-N 2 @C) were synthesized via calcinating straw biomass, which showed remarkable catalytic efficiency towards sulfamethoxazole (SMX) oxidation even under high-salinity conditions. Results and further elucidated the 1 O 2 formation pathway, where the Cu-N 2 sites adsorbed and interacted the oxygen atom in S O group at the end of peroxymonosulfate (PMS) with lower adsorption energy. This process was accompanied by the generation of two SO 5 •− molecular intermediates, ultimately leading to the formation of 1 O 2 with the lowest energy barrier. Moreover, toxicity tests showed that the degraded SMX solution was ecologically safe with no significant toxic effects on zebrafish, rice and Escherichia coli ( E. coli ). This study provides atomic-level insights into 1 O 2 generation via Cu-N 2 coordination, advancing the design of efficient and environmentally benign Fenton-like systems for antibiotic wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhangsong Jiang,Xiangfeng Huang,Qiaofeng Wu,Mi Li,Qili Xie,Zuwen Liu,Xiaoming Zou
Although microplastics (MPs) and sulfonamides (SAs) are emerging aquatic pollutants, the structural effects of SAs following their adsorption on MPs and underlying mechanisms of the same remain unelucidated. In this study, the characteristics of the adsorption of 10 SAs on polyamide (PA) were analyzed, and significant structural effects of the former were observed at different pH values (P < 0.01). The highest adsorption distribution coefficient ( K d ) was ∼7.83–43.57 times the lowest one. The key processes and micromechanisms of SA adsorption on PA were revealed using the quantitative structure–activity relationship model and partial least squares structural equation model (PLS-SEM). The results suggest that both the octanol–water partition coefficients ( K ow ) of SAs and the valid adsorption energies ( E ad-v ) between PA and SAs are vital in the observed structural effects of SAs. Furthermore, the density functional theory results demonstrated that during the adsorption of SAs on PA, the different adsorption energies were engendered by equilibrium configurations and interactions, such as hydrophobic, hydrogen bond (H-bond), van der Waals, and electrostatic interactions. Moreover, the developed PLS-SEM models revealed that during the adsorption of cationic (PA–SA + ) and anionic (PA–SA − ) SAs, the structural effects were partially driven by the electrostatic interactions. Conversely, the structural effects of neutral SA (SA 0 ) adsorption on PA were partially due to H-bond interactions. Overall, we pioneered a theoretical basis to understand the structural effects of SAs following their adsorption on MPs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Meng Xie,Mingya Yao,Shiyong Zhang,Lingshuai Kong,Lingxi Zhao,Jinhua Zhan,Ru-Song Zhao
Carbon-based single-atom cobalt catalysts exhibit high catalytic activity for the removal of novel pollutants in advanced oxidation processes. Here, atomically dispersed Co species with five-coordinated nitrogen atoms on carbon nanotubes (CNT) catalyst (Co-N 5 /CNT) was successfully fabricated via a low-temperature solvothermal reaction. The obtained Co-N 5 /CNT catalyst exhibited superior catalytic performance for PMS activation for sulfamerazine degradation. Its apparent rate constant k obs was 1.6 times higher than that of the Co-N 4 /CNT catalyst with four-coordinated nitrogen atoms prepared by the same method. Electron transfer non-radical mechanism was the main pathway for Co-N 5 /CNT to activate PMS. Higher single-atom cobalt metal loading (1.39 wt% vs 1.08 wt% in Co-N 4 /CNT) and significantly enhanced electron transfer ability (0.82 e vs 0.77 e in Co-N 4 /CNT) were the key factors for its superior catalytic performance. This work demonstrates a novel carbon-based single-atom cobalt catalyst for the removal of novel antibiotic contaminants by activating PMS in environmental catalysis applications.
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MOLECULES
·
2023
·Vol. 28
·期 4
·1541
·
IF 4.6
Pascaline Sanga,Juanjuan Wang,Xin Li,Jia Chen,Hongdeng Qiu
Developing a simple and efficient method for removing organic micropollutants from aqueous systems is crucial. The present study describes the preparation and application, for the first time, of novel MXene-decorated bismuth ferrite nanocomposites (BiFeO3/MXene) for the removal of six sulfonamides including sulfadiazine (SDZ), sulfathiazole (STZ), sulfamerazine (SMZ), sulfamethazine (SMTZ), sulfamethoxazole (SMXZ) and sulfisoxazole (SXZ). The properties of BiFeO3/MXene are enhanced by the presence of BiFeO3nanoparticles, which provide a large surface area to facilitate the removal of sulfonamides. More importantly, BiFeO3/MXene composites demonstrated remarkable sulfonamide adsorption capabilities compared to pristine MXene, which is due to the synergistic effect between BiFeO3and MXene. The kinetics and isotherm models of sulfonamide adsorption on BiFeO3/MXene are consistent with a pseudo-second-order kinetics and Langmuir model. BiFeO3/MXene had appreciable reusability after five adsorption–desorption cycles. Furthermore, BiFeO3/MXene is stable and retains its original properties upon desorption. The present work provides an effective method for eliminating sulfonamides from water by exploiting the excellent texture properties of BiFeO3/MXene.Keywords:MXene;bismuth ferrite;nanocomposite;sulfonamide;adsorption
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Journal of Environmental Sciences
·
2022
·
IF 6.796
Jie Du,Zhijun An,Yufeng Hu,Xianliang Yi,Hao Zhou,Jingjing Zhan,Minghuo Wu
Sulfonamides (SAs) are one of the most widely used antibiotics and their residuals in the environment could cause some negative environmental issues . Advanced oxidation such as Fenton-like reaction has been widely applied in the treatment of SAs polluted water. Degradation rates of 95%-99.7% were achieved in this work for the tested 8 SAs, including sulfisomidine, sulfameter (SME), phthalylsulfathiazole, sulfamethoxypyridazine, sulfamonomethoxine, sulfisoxazole, sulfachloropyridazine, and sulfadimethoxine, in the Fe 3 O 4 /peroxodisulfate (PDS) oxidation system after the optimization of PDS concentration and pH. Meanwhile, it was found that a lot of unknown oxidation products were formed, which brought up the uncertainty of health risks to the environment, and the identification of these unknown products was critical. Therefore, SME was selected as the model compound, from which the oxidation products were never elucidated, to identify these intermediates/products. With liquid chromatography-high resolution tandem mass spectrometry (LC-HRMS/MS), 10 new products were identified, in which 2-amino-5-methoxypyrimidine (AMP) was confirmed by its standard. The investigation of the oxidation process of SME indicated that most of the products were not stable and the degradation pathways were very complicated as multiple reactions, such as oxidation of the amino group, SO 2 extrusion, and potential cross-reaction occurred simultaneously. Though most of the products were not verified due to the lack of standards, our results could be helpful in the evaluation of the treatment performance of SAs containing wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhuo-Rui Jiang,Pengfei Wang,Yu-Xiao Zhou,Changhua Wang,Jiwen Jiang,Yeqing Lan,Cheng Chen
An elastic and 3D-blocky catalyst (CoMnO x @sponge) was successfully prepared via uniform growth and distribution of Co-Mn bimetallic oxide inside the sponge for the activation of peroxymonosulfate (PMS). The results showed that 30 mg/L sulfisoxazole (SIZ) could be completely degraded by PMS (1 mM) activated with CoMnO x @sponge (0.1 g/L) within 5 min. The pseudo-first-order rate constant was calculated to be 1.83 min −1 , which was much larger than those from previous reports. The excellent stability and reusability of CoMnO x @sponge were confirmed through 20 recycle runs with more than 90% degradation of SIZ and less than 0.9 mg/L leached metal ions. Singlet oxygen ( 1 O 2 ), hydroxyl radicals ( • OH) and sulfate radicals (SO 4 •− ) were determined to be the dominating reactive oxygen species (ROS) responsible for the degradation of SIZ. The possible pathways of SIZ degradation as well as underlying catalytic mechanism were deduced. The bio-toxicity declined obviously after the mineralization of SIZ and the removal of TOC at 5 mg/L SIZ was high up to 90.4%. Furthermore, the system of CoMnO x @sponge/PMS also exhibited the strong anti-interference ability in natural water and the universal degradation capacity towards other common organic pollutants. More remarkably, the 3D-catalyst possessing an elasticity and extremely high porosity could be easily assembled with a column to realize the consecutive degradation of pollutants. The labor- and time-saving removal of pollutants based on a combination of CoMnO x @sponge with PMS makes it great potential in practical application.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Honglong Zhang,Zhenyu Shi,Jun Ma,Fuyi Cui,Jing Zhang,Timothy J. Strathmann
In this study, a representative redox mediator, 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO), and its para-substituted derivatives (TEMPOs: 4-hydroxyl-TEMPO, 4-acetylamino-TEMPO, and 4-amino-TEMPO) significantly accelerated the abatement of trace organic contaminants (TrOCs, i.e., bisphenol-A (BPA), phenol, amines, and phenylbutazone) by Mn(VII) over a wide pH range of 4.0–9.0. The addition of substituents at para to the > N–O• moiety significantly influenced the degradation kinetics of TrOCs by changing the reduction potentials of TEMPOs and the corresponding oxoammonium cations (TEMPOs+); a linear relationship was observed between the substituents’ para Hammett sigma constants and the reduction potentials of TEMPOs and TEMPOs+. Pseudo-first-order reaction rate constants (kobs, min–1) of TrOC degradation by Mn(VII)/TEMPOs were also affected by the pKa of the TrOCs. Generally, the highest kobs values for individual TrOCs were observed at pH near the pKa even for TEMPOs+ with relatively pH-invariant reduction potentials. Overall, TrOC abatement kinetics were related to a combination of reactive species (Mn(VII), in situ formed MnO2, and TEMPOs+). For BPA, the relative contributions (R) of reactive species ranked as R(TEMPOs+) > R(Mn(VII)) > R(in situ formed MnO2) at pH 4.0–8.0, whereas R(Mn(VII)) > R(TEMPOs+) at pH 9.0 mainly owing to a change in BPA speciation as the pH approached the pKa1 value for BPA. The results of this study are useful for the development of heterogeneous TEMPO-based redox mediators and future applications of TEMPO-mediated oxidation systems for accelerated abatement of TrOCs in water.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Yuhan Ning,Yixing Ye,Wanliang Liao,Yang Xu,Weiping Wang,Ai-jun Wang
In this work, triazine-based porous organic polymer (TAPT-BPDA) synthesized by simple solvothermal method with stable chemical properties was employed as pipette tip solid-phase extraction (PT-SPE) adsorbent for the extraction of sulfonamides for the first time. Under the optimal conditions, good linearities (1–300 μg L −1 , R 2 ≥ 0.9987) and low limits of detection (0.10–0.28 μg L −1 ) were obtained. The recoveries of sulfonamides in meat, egg and milk samples were in the range of 76.1–114.0 %. The prepared TAPT-BPDA showed good reusability with the recoveries of sulfonamides remained above 80.0 % after eight recycles. The adsorption mechanism between SAs and adsorbent might be the combined effects of electrostatic interactions, hydrogen bonding and π-π interactions. The results demonstrated potential applications of a TAPT-BPDA-based PT-SPE-HPLC method for the analysis of trace sulfonamide residues in food samples.
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ACS Agricultural Science & Technology
·
2021
·
IF 0
Mi Li,Xiaoyu Xiao,Zhangsong Jiang,Haihui Tang,Lingling Rong,Tiao Zhang,Taijia Li,Cui Hu,Ligui Wu,Xiaoming Zou
Antibiotic resistance genes (ARGs) are emerging environmental pollutants, and the effect of both abiotic (e.g., anthropogenic pollutants such as sulfonamides (SAs)) and biotic (e.g., microbial community (taxonomy), mobile genetic elements (MGEs)) factors on the antibiotic resistome (collection of ARGs) has received much attention recently. In addition, function (e.g., CAZy, eggNOG and KEGG) is also an important biotic factor; however, how function correlates to ARGs and thus contributes to the antibiotic resistome remains ambiguous. This work explores the effect of sulfonamides (SAs) on ARGs and MGEs by a metagenomic analysis, a principal component analysis (PCA), and a nonmetric multidimensional scaling analysis (NMDS). Then, the work establishes a correlation between ARGs and function with a co-occurrence network and reveals the contribution and positive (negative)/direct (indirect) effect of taxonomy, MGEs, and function to the antibiotic resistome by variation partitioning analysis (VPA) and partial least-squares-path modeling (PLS-PM). The results show that the soil has diverse ARGs and several MGEs and SAs impose significant effects on them. Further, CAZy, eggNOG, and KEGG (including pathway and orthology) show strong and significant correlation with ARGs on the basis of the co-occurrence network; however, in our system it seems that only the KEGG pathway promotes the interpretation of ARGs and should be regarded as the priority function on considering the role of function in structuring the antibiotic resistome. This work reveals the importance and necessity of function as a biotic factor in shaping the antibiotic resistome in diverse resistome-related fields.
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LANGMUIR
·
2021
·
IF 3.882
Yu Wang,Jia Chen,Ming Guan,Hongdeng Qiu
An iron–nickel bimetallic oxide porous graphene composite material (Fe/Ni-PG) was prepared by a simple partial combustion method, which can be used to effectively remove sulfonamides (SAs) from an aqueous solution. The adsorption performance of Fe/Ni-PG, Fe-PG, and Ni-PG on six kinds of SAs was compared, and the influence of time, temperature, pH, and initial concentration of SAs on the adsorption behavior of SAs of Fe/Ni-PG in an aqueous solution was studied. The adsorption kinetics and thermodynamics exhibited that the Langmuir model and pseudo-second-order kinetics model can describe the adsorption isotherm and kinetics. The maximum adsorption capacities of sulfadiazine (SD), sulfamerazine (SM), sulfamethazine (SDM), sulfathiazole (STZ), sulfapyridine (SPD), and sulfisoxazole (SIZ) calculated by the Langmuir model were 26.3, 50.3, 42.2, 27.3, 34.5, and 41.7 mg/g, respectively, which exceeded those of most reported adsorbents. In the adsorption process, hydrogen bonding, π–π electron donor–acceptor, electrostatic interaction, and bimetallic synergies play a major role, and the entire adsorption process is spontaneously endothermic. In addition, the material has excellent stability, and the Fe/Ni-PG after desorption is consistent with the raw material. This work provides a favorable way for the removal of SAs in the environment.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 10
·1-11
·
IF 5.833
Qin
Peige,Han Lizhen,Zhang Xiaowan,Li Mengyuan,Li Dan,Lu Minghua,Cai Zongwei
Abstract Using MIL-101(Fe) as the source of carbon and Fe, a magnetic porous carbon (MPC) material with Fe 3 C nanoparticles encapsulated in porous carbon was prepared through one-pot pyrolysis under N 2 atmosphere. With MPC as adsorption material, a stir bar sorptive-dispersive microextraction (SBSDME) method was proposed to extract and preconcentrate sulfonamides (SAs) prior to HPLC-DAD determination. To investigate their extraction ability, different MPC materials were prepared under different carbonization temperatures (600, 700, 800, 900, and 1000 °C). The material prepared under 900 °C (MPC-900) exhibited the highest extraction ability for SAs. The as-prepared MPC materials were also characterized by Raman spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, zeta potential, and other techniques. The main parameters that affect extraction were systematically studied. Under optimal conditions, favorable linearity ( R 2 ≥ 0.9938) and detection limits (0.02–0.04 ng mL −1 ) of sulfonamides were obtained. The average recoveries for spiked milk and lake water samples ranged from 76.9 to 109% and from 75.4 to 118% with RSDs of 3.10–9.63% and 1.71–11.3%, respectively. Sulfameter and sulfisoxazole were detected in milk sample. Sulfisoxazole was detected in the lake water sample. The MPC-900 material demonstrated excellent reusability. It can be reused 24 times with peak areas having no obvious decline. The method can be applied to extract ultra-trace compounds in complex sample matrices. Graphical abstract
Schematic presentation of a stir bar sorptive-dispersive microextraction (SBSDME) by using magnetic porous carbon (MPC) composites as sorbent combined with high-performance liquid chromatography for sensitive analysis of sulfonamides in milk and lake water samples.
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WATER RESEARCH
·
2021
·
IF 11.236
Chenying Zhou,Peng Zhou,Minglu Sun,Yang Liu,Heng Zhang,Zhaokun Xiong,Juan Liang,Xiaoguang Duan,Bo Lai
The sluggish kinetics of Fe(II) recovery strongly impedes the scientific progress of Fenton reaction (Fe(II)/H 2 O 2 ) towards practical application. Here, we propose a novel mechanism that metal-free nitrogen-doped carbon nanotubes (NCNT) can enhance Fenton chemistry with H 2 O 2 as electron donors by elevating the oxidation potential of Fe(III). NCNT remarkably promotes the circulation of Fe(III)/Fe(II) to produce hydroxyl radical ( • OH) with excellent stability for multiple usages (more than 10 cycles) in the NCNT/Fe(III)/H 2 O 2 system. Although carbonyl on NCNT can act as the electron supplier for Fe(III) reduction, the behavior of NCNT is distinct from common reductants such as hydroxylamine and boron. Electrochemical analysis and density functional theory calculation unveil that nitrogen sites of NCNT can weakly bind with Fe(III) to elevate the oxidation potential of Fe(III) (named near-free Fe(III), primarily FeOH 2+ ) at pH ranging from 2.0 to 4.0. Without inputs of external stimulations or electron sacrificers, near-free Fe(III) can promote H 2 O 2 induced reduction of Fe(III) to initiate Fenton chain reactions for long-lasting generation of • OH. To our delight, it is a common property of N-doped carbon materials (e.g., graphene, carbon nanofibers, and acetylene black), our research thus provides a novel, sustainable, and green strategy for promoting Fenton chemistry.
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