CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Shilan Zhang,Songsong Zhi,Hongju Wang,Jing Guo,Weihao Sun,Lu Zhang,Yi Jiang,Xiaguang Zhang,Kai Jiang,Dapeng Wu
A solid-state laser scanning treatment (SLST) was adopted to synthesize anatase/rutile TiO 2 heterojunction with effective charge carrier separation and high surface adsorption performances for the photodegradation of sulfamethoxazole (SMX). The 1064 nm pulsed fiber laser could in-situ generate rutile zones on the pristine sheet-like anatase crystal enclosed by (0 0 1) facets, which could form the well-defined anatase/rutile interface to promote the formation of dominating active species ( h + and ∙OH) on the anatase zones. X-ray absorption fine structure (XAFS) measurements, low temperature electron paramagnetic resonance (LT-EPR) as well as the density functional theory (DFT) simulation proved that the oxygen vacancies (V O ) could both introduce defective energy states to promote the light absorption and enhance the SMX adsorption on anatase zones. Based on the delicately designed micro-zones, the photodegradation efficiency of the optimized catalyst could reach 99.3 %, which demonstrated ∼7 times higher performance than that of pristine TiO 2 and exhibited robust stability under environmental conditions. Gaussian and Vienna Ab Initio Package (VASP) programs were used to provide detailed degradation pathways and mechanism for SMX. This SLST could be potentially employed to create function-specified zones on various catalysts for different applicational aims.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Xintao Fu,Yan Lin,Chunping Yang,Shaohua Wu,Yue Wang,Xiang Li
Transition-metal phosphides (TMPs) have been considered a promising candidate for heterogeneous catalysis in wastewater treatment , while the feasibility of its application in peroxymonosulfate (PMS) based advanced oxidation processes systems for the treatment of high-salinity organic wastewater remains still unclear. In this study, catalysts of cobalt phosphide (CoP) nanoparticles confined in nitrogen-doped porous carbon (CoP/NC) were prepared using zeolitic imidazolate framework-67 (ZIF-67) as a template via calcination-oxidation-phosphorization, which were subsequently applied to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX) in the water with high-salinity concentrations. Results showed that the degrading performance of CoP/NC could be improved and regulated by phosphorus (P) doping amount with an optimum of 5.0% (CoP/NC-5), which reached 100% of SMX degradation. Meanwhile, CoP/NC-5 catalyst could tolerate wide pH variations (5–9). More importantly, the CoP/NC-5/PMS system showed high adaptability to various concentrations of inorganic salt, even up to 500 mM. In addition, active species of sulfate radical (SO 4 •− ) and singlet oxygen ( 1 O 2 ) were identified, which played dominant roles in the destruction of SMX, and the production amount of SO 4 •− was quantified. This work confirmed that transition-metal phosphides nanoparticles confined in nitrogen-doped porous carbon were a promising catalyst for SMX elimination in high saline wastewater.
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CHEMOSPHERE
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2023
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IF 8.8
Kai Wang,Xiaojiao Yu,Zongbin Liu,Ting Zhang,Yao Ma,Jinfen Niu,Binhua Yao
Constructed heterojunction has been considered an efficient strategy to enhance the migration and transfer of photoinduced charge carriers. Herein, a Z-scheme Cu 2 O/BiOBr heterojunction with 0D/2D structure was fabricated by microwave hydrothermal method. It was found that the optimal composites photocatalyst showed excellent activity for sulfamethoxazole (SMZ) illumination, and the removal rate reached 90.7%, which was higher than pristine Cu 2 O (53.0%) and BiOBr (60.0%). Subsequently, the operational parameters such as catalyst dosage, concentrations of pollutants, and pH of solution were investigated. According to the ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRs), Mott-Schottky curve, and density functional theory (DFT) analysis, the Z-scheme degradation mechanism of Cu 2 O/BiOBr heterostructure was proposed. Among them, the interface structure of 0-dimensions/2-dimensions (0D/2D) can significantly increase the number of heterojunctions in the composite catalyst, and Z-scheme heterostructures can accelerate the generation and migration of photoinduced charge carriers, which has a facilitation effect on improving the decomposition activity of the photocatalyst. Moreover, three possible pathways for SMZ degradation were inferred. This study provides a promising strategy for constructing novel heterojunctions with high photocatalytic performance.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Shizong Wang,Jianlong Wang
High efficient activator is highly desired in the field of persulfate-based advanced oxidation process. In comparison with the previous studies, this study adopted nitrogen, sulfur and oxygen co-doped carbon material to support Fe 0 encapsulate in Fe 3 O 4 to prepare iron-based modified carbon composite (Fe 0 @Fe 3 O 4 -MC) by a facile two-step pyrolysis. Fe 0 @Fe 3 O 4 -MC was then used for degradation of sulfamethoxazole. The results showed that Fe 0 @Fe 3 O 4 -MC had superior catalytic activity for PMS activation due to the synergistic effect of iron-based compound and modified carbon. In the presence of 0.1 g/L of Fe 0 @Fe 3 O 4 -MC, SMX (0.04 mM) could be completely degraded within 120 min at pH 3.4 and 3 mM of PMS. The SMX degradation followed pseudo first-order kinetic model, with the rate constant of 0.12 min −1 , and the mineralization of SMX achieved 48.4%. Sulfate radicals dominated in the SMX degradation. In addition to Fe 0 and Fe 3 O 4 , carbon defects, graphitic N, sulfur and FeN 4 also contributed to PMS activation. Fe 0 oxidation was the rate-limiting step for PMS activation. Dissolved oxygen made a minor contribution to Fe 0 oxidation. The intermediate products of SMX degradation were identified, and two pathways of SMX degradation were proposed. The influencing factors on SMX degradation were studied, including pH, temperature, PMS concentration, Fe 0 @Fe 3 O 4 -MC dosage, chloridion, carbonate and humic acids, and the influencing mechanism was discussed. This study could provide an efficient PMS activator for the degradation of emerging organic pollutants in water and wastewater.
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EUROPEAN JOURNAL OF PHARMACEUTICAL SCIENCES
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2021
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IF 4.384
Ling-Yang Wang,Fan-Zhi Bu,Yue-Ming Yu,Yuan-Yuan Niu,Yan-Tuan Li,Cui-Wei Yan,Zhi-Yong Wu
In order to exploit the advantages to the full of multidrug salification strategy in amending the pharmaceutical properties of drugs both in vitro and in vivo , and further to open up a new way for its applications in bacteria-virus mixed cross-infection drugs, a novel dual-drug crystalline molecular salt hybridizing antibacterial drug sulfamethoxazole (SFM) with antiviral ingredient amantadine (ATE), namely SFM-ATE, is successfully designed and synthesized via multidrug salification strategy oriented by proton exchange reaction. The crystal structure of the firstly obtained molecular salt is precisely identified by employing single-crystal X-ray diffraction and multiple other techniques. The results show that, in the crystal lattice of molecular salt SFM-ATE, the classical hydrogen bonds together with charge-assisted hydrogen bonds contribute to two- dimensional networks, between which the hydrophobic interaction plays an important role. The relevant in vitro/vivo pharmaceutical properties of the dual-drug molecular salt are carried out through a comparative investigation of theoretical and experimental methods. It has been found that SFM displays concurrent improvements over the bulk drug in its permeability and dissolution after forming the molecular salt, which is supported by the molecular electrostatic potential calculation and Hirshfeld surface analysis. Encouragingly, the perfected in vitro biopharmaceutical properties can effectually turn into the in vivo pharmacokinetic preponderances with the expedited peak plasma concentration, lengthened half-life and enhanced bioavailability. Better yet, the antibacterial activities of SFM from the molecular salt get stronger with enlargement in inhibition areas and reduction in values of minimum inhibitory concentrations against the tested bacterial strains. Consequently, the present contribution not only supplies an opportunity for widening applications for classical sulfa drugs via dual-drug salification strategy, but also offers an alternative approach in dealing with viral-bacterial coinfection even other complex diseases by drugs’ hybridization at the molecular level.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Junlei Zhang,Wei Zhao,Zhi Li,Gang Lu,Mingshan Zhu
Advanced oxidation processes involving the visible-light-assisted peroxymonosulfate (PMS) are emerging as promising approaches for treating antibiotic pollutants. Here, Fe(II)/V(IV) self-doped FeVO 4 nanobelts were synthesized and employed to build a visible-light-assisted PMS activation system for degrading antibiotic sulfamethoxazole (SMX). Compared with PMS/FeVO 4 , PMS/Visible light (VL), or PMS system, the PMS/FeVO 4 /VL system showed 3.9, 14.0, or 14.1 times improved for the removal of SMX, respectively. The reason behind this is the organic combination of the VL photocatalysis and transformation of Fe(II)/V(IV) to Fe(III)/V(V) over FeVO 4 , namely when photocatalytic behavior over FeVO 4 can produce electrons (e - ) and holes (h + ) to activate PMS or directly degrade SMX, the transformation of Fe(II)/V(IV) to Fe(III)/V(V) will also happen to donate some e - for PMS activation simultaneously. Such a system can also effectively remove SMX from actual water bodies such as medicine wastewater, river water, tap water, and rainwater. This work not only provides an effective system for treating SMX polluted wastewater, but also gives some new insights to understanding the mechanism involving Fe-based binary metal oxide activating peroxymonosulfate.
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ADSORPTION SCIENCE & TECHNOLOGY
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2020
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IF 2.425
Tian Ai,Xiaojun Jiang,Zhenxia Zhong,Dachao Li,Shujuan Dai
The efficient capture of drug metabolites from aquatic environments has been recognized as an essential task for environmental protection. A methanol-modified ultra-fine magnetic biochar (CH3OH-OP-char/Fe3O4) was prepared from orange peel powder using ball milling, and its adsorption behaviors for ibuprofen and sulfamethoxazole were evaluated. The obtained materials were characterized by laser particle size analyzer, EA, ICP-OES, VSM, BET, TG-DTG, and FTIR. Furthermore, the experiments were conducted to study the vital operating parameters such as solution pH (2.0–11.0), contact time (0.5–240 min), initial drug concentration (0.5–100 mg/L), and temperatures (15–40°C) on the removal process. The results showed that the adsorption of IBP and sulfamethoxazole on CH3OH-OP-char/Fe3O4 was highly pH-dependent. Kinetic studies indicated that physisorption was the dominant adsorption mechanism, and film diffusion played a vital role in adsorption onto CH3OH-OP-char/Fe3O4. Equilibrium data were fitted well with the Langmuir isotherm model, implying monolayer adsorption. The adsorption process was spontaneous and endothermic due to the thermodynamic calculation, and high temperatures were favorable to the adsorption process.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Haiqiang Qi,Xiuping Sun,Zhirong Sun
Bifunctional electrodes have attracted significant research interest in the field of heterogeneous electro-Fenton (hetero-EF) process for efficient treatment of antibiotic-containing wastewater. In this study, etched graphite felt (EGF) was used as the matrix material because of its excellent electrochemical properties, rich pore structure, and large specific surface area. The transition metals Cu and Fe were in situ grown on the EGF electrode surface without polymer binder by a one-step hydrothermal method. The obtained electrode consisting of Cu-doped Fe 2 O 3 nanoparticles/EGF (Cu-Fe 2 O 3 /EGF) was used in the hetero-EF process for in situ electro-generation and activation of hydrogen peroxide (H 2 O 2 ) for efficient degradation of sulfamethoxazole (SMX). The Cu-Fe 2 O 3 /EGF electrode demonstrated a wide pH application range of 3.0–9.0. According to electron spin resonance and free-radical quenching experiments, hydroxyl radical and superoxide anion were the dominant species in the hetero-EF process, while the hydroxyl radical played a major role in the degradation of SMX. In consecutive runs, the electrode exhibited low metal ion leaching and excellent stability. Furthermore, the possible mechanism for the production and activation of H 2 O 2 as well as possible SMX degradation pathways were proposed. The toxicity of SMX samples during degradation exhibited a decreasing trend according to the results of toxicological simulation and Escherichia coli growth test. This study provides a new strategy for the construction of an efficient and stable bifunctional cathode for the advanced treatment of antibiotic-containing wastewater.
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WATER RESEARCH
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2019
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IF 7.913
Tian-Yang Zhang,Bin Xu,Shijie Yao,Yaru Hu,Kuangfei Lin,Hui Ye,Changzheng Cui
Pre-chlorination and UV disinfection are two common processes in drinking water treatment plants. Sulfamethoxazole (SMX), an antibiotic widely detected in source water, was selected as a precursor to study the conversion of chlorine/nitrogen species and DBP formation in pre-chlorination/post-UV process. The combined chlorine (mainly organic chloramines) produced in pre-chlorination of SMX can self-degrade and release free chlorine back again as pre-chlorination time goes on. With free chlorine dose increasing, the self-degradation rate of combined chlorine increased obviously. But the combined chlorine stopped self-degrading and remained stable around 1 mg-Cl 2 /L after adding 0.30 mM chlorine for 30 min. Post-UV treatment after pre-chlorination can enhance the degradation and achieve a complete removal of combined chlorine (including organic chloramines). Deamination occurred during pre-chlorination/post-UV process and deamination amount (-NH 2 ) per SMX concentration was 0.19 M/M. Radicals in this process had no obvious influence on chlorine/nitrogen species conversion. Direct chlorination of SMX had the lowest DBP formation potentials while the application of pre-chlorination and UV enhanced them. Compared with UV treatment only, dichloroacetonitrile formation potential of SMX reduced by 1.58 × 10 −3 mol/mol-SMX (17.37 μg/l) after pre-chlorination/post-UV treatment. During pre-chlorination/post-UV/final-chlorination treatment of SMX, Br − and natural organic matter can enhance DBP formation and toxicity-weighted values. Acid conditions showed a very high DBP risk, while alkaline conditions could cut this risk obviously, especially for the toxicity-weighted values of these DBPs.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Si Li,Ruizhe Xu,Luochao Wan,Chaomeng Dai,Jixiang Li,Xueji You,Yanping Duan,Xiaoying Lai,Zhi Li,Jifeng Guo,Yalei Zhang,Jiajun Hu,Lang Zhou,Xiaoyi Huang
This study examines the efficacy and environmental impact of peracetic acid (PAA) activated by thermally modified activated carbon (AC600) for degrading antibiotics in actual groundwater. Laboratory-scale experiments evaluated the system's effects on contaminant degradation, ecological balance, and substance cycling in the hyporheic zone. Our findings demonstrated the effectiveness of the AC600/PAA system in removing sulfamethoxazole (SMX) from groundwater porous media. Additionally, the AC600/PAA system synergistically interacted with the in-situ microbiota of the hyporheic zone, producing more fragmented degradation products without increasing mixed toxicity. Bacterial abundance increased post-reaction, with notable alterations in the bacterial community and enhanced bacterial metabolism. Key genera such as Lysobacter thrived in the treated environment, playing critical roles in microbiota modification and SMX degradation. The pH remained stable before and after the reaction, while dissolved organic carbon content increased. Overall, our results highlight the promising potential of PAA activation by carbonaceous materials as a low-impact, ecologically friendly technology for in-situ remediation of organic pollutants in groundwater, characterized by high compatibility and biosynthesis.
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Journal of Water Process Engineering
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2024
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IF 6.3
Wei Gao,Huide Chen,Xiaowei Liu,Ling Zhang,Haitao Ding,Chengxun Deng
The synthesis of biochar-based catalysts from bamboo strip biomass waste aligns with the principles of environmental sustainability and recycling. This study focuses on the degradation of sulfamethoxazole (SMX) in a simulated aqueous environment. A composite catalyst (IC–BC) was prepared by impregnating bamboo strip biochar (BC) with iron concentrates (IC). The optimal configuration for the oxidative degradation of SMX was achieved using IC-BC-activated persulfate (PS). The structural, morphological, optical, and electrochemical properties of the IC-BC were thoroughly characterized, revealing its robust stability through repeated cycles. The dielectric barrier discharge (DBD) synergistic IC-BC/PS oxidation system demonstrated an SMX degradation efficiency of 93.33 % in 10 min. Quenching experiments and electron paramagnetic resonance (EPR) spectroscopy identified radicals O• − 2 , • OH, and SO• − 4 radicals as the primary active species involved in the degradation process. Ultraviolet-visible absorption spectroscopy (UV–Vis) confirmed this synergistic effect. Liquid chromatography mass spectrometry (LC-MS) identified four potential SMX degradation pathways. Total Organic Carbon (TOC) elimination efficiency tests and toxicological analyses revealed that the intermediates were significantly less toxic than SMX. These results demonstrate that the DBD/IC-BC/PS system significantly enhances the removal efficiency of SMX, offering excellent environmental protection properties.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yuxin Qi,Ying Bi,Chao Kong,Changyin Zhu,Hu Cheng,Yinlong Zhang,Jiangang Han,Jianming Xue,Ziyan Li,Yang Song,Dongmei Zhou
Recycling difficult-to-degrade plastics, also known as “white pollution”, is currently being researched in the fields of materials and the environment, which is an extremely challenging topic. In this study, a pyrolysis-activation method combined with multiple activators was developed to prepare stable porous plastic chars (PPCs) from discarded plastic bottles for removing the typical antibiotic sulfamethoxazole (SMX). Micro/mesopores were formed in the PPCs, with the specific surface area reaching 961.20 m 2 /g. C, O, and N were the main elements in the PPCs, and their atomic ratios showed the hydrophobicity and aromaticity. Graphite-like structures and abundant surface functional groups were generated in the PPCs. Unlike conventional char materials, impurities, such as aluminum oxide, have high reflectivity, resulting in the appearance of many shining spots. PPCs display a high sorption capability for SMX, with the maximum sorption quantity determined reaching 487.52 mg/g. Multilayer sorption is dominated by physical processes, and pore filling, partitioning, hydrogen bonding, π-π stacking, and electrostatic interactions are the main sorption processes. Chemical-like sorption and mass transfer control the sorption rate. Furthermore, PPCs have stable performance and good recyclability and could be used for practical applications. This study provides a novel strategy and an example of the upcycling of discarded plastic as an excellent char material for environmental remediation.
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