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ENVIRONMENTAL RESEARCH · 2023 · IF 8.3

Enhanced sulfamethazine detoxification by a novel BiOCl (110)/NrGO/BiVO4 heterojunction

Xiaofan Yang,Yutao Xu,Saraschandra Naraginti,Xueyu Wei

The emerging contaminants removal from the environment has recently been raised concerns due to their presence in higher concentrations. Over usage of emerging contaminant such as sulfamethazine poses serious threat to the aquatic and human health as well. This study deals with rationally structured a novel BiOCl (110)/NrGO/BiVO 4 heterojunction which is used to detoxify sulfamethazine (SMZ) antibiotic efficiently. The synthesised composite was well characterized and the morphological analysis evidenced the formation of heterojunction consisted of nanoplates BiOCl with dominant exposed (110) facets and leaf like BiVO 4 on NrGO layers. Further results revealed that the addition of BiVO 4 and NrGO tremendously increased the photocatalytic degradation efficiency of BiOCl with the rate of 96.9% (k = 0.01783 min −1 ) towards SMZ within 60 min of visible light irradiation. Furthermore, heterojunction energy-band theory was employed to determine the degradation mechanism of SMX in this study. The larger surface area of BiOCl and NrGO layers are believed to be the reason for higher activity which facilitates the excellent charge transfer and improved light absorption . In addition, SMZ degradation products identification was carried out by LC-ESI/MS/MS to determine the pathway of degradation. The toxicity assessment was studied using E. coli as a model microorganism through colony forming unit assay (CFU), and the results indicated a significant reduction in biotoxicity was observed in 60 min of degradation process. Thus, our work gives new methods in developing various materials that effectively treat emerging contaminants from the aqueous environment.

研究领域: 环境科学 · 材料科学 · 毒理学
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

High-efficiency and stable Z-scheme heterojunction of Co9S8 anchored by g-C3N4 for peroxymonosulfate activation

Yao Lu,Mengjie Fu,Cheng Cheng,Haocheng Yang,Xinyi Ni,Jiayuan Guo,Shihai Cao

Photocatalytic technology and peroxymonosulfate (PMS) based advanced oxidation technology have been proven to be simple and effective strategies for recalcitrant organic pollutants degradation. In this work, we designed and prepared a coupled photocatalytic and advanced oxidation system for sulfamethazine (SMR) antibiotics degradation. Firstly, a series of Z-scheme Co 9 S 8 /g-C 3 N 4 heterojunction photocatalysts are prepared by a simple two-step method and further work as PMS activators. The prepared Co 9 S 8 /g-C 3 N 4 photocatalysts exhibit a great improvement in electron-hole pairs migration and visible-light response due to heterojunction formation. In addition, the g-C 3 N 4 acts as a substrate to anchor the Co 9 S 8 nanoparticle, which suppresses the Co 9 S 8 leaching and prevents the Co 9 S 8 oxidation. Consequently, the Co 9 S 8 /g-C 3 N 4 /PMS system displayed an improved SMR degradation ability (93 % for Co 9 S 8 /g-C 3 N 4 /PMS vs. 86 % for Co 9 S 8 /g-C 3 N 4 ). After the fourth cyclic degradation experiment, the Co 9 S 8 /g-C 3 N 4 /PMS system still maintained a comparatively high degradation rate. Considering its good properties and better degradation performance, we propose that the synergistic effect of photocatalytic technology and PMS possess a promising prospect for application in environmental treatment.

研究领域: 环境科学 · 材料科学
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Catalysts · 2023 ·Vol. 13 ·期 1 ·172 · IF 3.9

Construction of Multi-Defective ZnMn2O4/Carbon Nitride Three-Dimensional System for Highly Efficient Photocatalytic Sulfamethoxazole Degradation

Yandong Xu,Jianjun Liao,Linlin Zhang,Yakun Li,Chengjun Ge

Rational design of composite nanostructured photocatalytic systems with good sunlight absorption capacity and efficient charge separation and transfer ability is an urgent problem to be solved in photocatalysis research. Here, a ZnMn2O4decorated three-dimensional carbon nitride with O, C co-doping, and nitrogen defect composite photocatalytic system was prepared using a simple hydrothermal method and subsequent calcination method. For the photocatalytic reactions, the presence of heterostructures, C, O co-doping, and nitrogen defects greatly promotes the separation and transfer of charges at the semiconductor/semiconductor interface under the local electric field, thereby extending its service life. The photocatalytic degradation efficiency of sulfamethoxazole in water is as high as 94.3% under the synergistic effects, which is also suitable for the complex water environment. In addition, the synthesized photocatalyst has good chemical stability and recyclability. This study provides a new opportunity to solve the problem of environmental pollution.Keywords:multi-defective C3N4;ZnMn2O4;composite system;photocatalytic sulfamethoxazole degradation

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Surface-nucleated heterogeneous growth of zeolitic imidazolate framework – A unique precursor towards catalytic ceramic membranes: Synthesis, characterization and organics degradation

Yueping Bao,Wen-Da Oh,Teik-Thye Lim,Rong Wang,Richard David Webster,Xiao Hu

A novel Co 3 O 4 nanocatalyst functionalized Al 2 O 3 ceramic membrane (CoFCM) with a honeycomb structure was prepared via an optimized surface-nucleated zeolitic imidazolate framework (ZIF-67) growth method. The Co 3 O 4 hollow structure which was confirmed via chemical characterizations (XRD, FTIR, Raman and XPS), was formed on the membrane surface by one-step calcination of ZIF-67 membrane. The CoFCM was characterized by various techniques including the field emission scanning electron microscopy and atomic force microscopy. The results revealed the formation of well-defined Co 3 O 4 layer on the porous Al 2 O 3 ceramic membrane with the thickness of 1.5–2 µm. The growth mechanism of CoFCM was further proposed via XPS and the catalytic activity of CoFCM was investigated for the removal of sulfamethoxazole (SMX) with the addition of Oxone. The membrane performance was examined under a home-made dead-end mode. Results indicated that CoFCM has a rougher surface with an initial membrane resistance of 1.19 × 10 11  m −1 and performs outstanding catalytic activity. The pure water permeability of CoFCM is 3024 L m −2  h −1  bar −1 , which is comparable to that of the pristine ceramic membrane (<10% difference). The SMX removal efficiency achieved to >90% in 90 min with an Oxone addition of 0.1 g L −1 . Meanwhile, the membrane showed excellent durability by retaining >95% of initial flux for at least 3 operational cycles with a low cobalt ion leaching via Oxone-assisted cleaning. Furthermore, the reaction mechanism of Oxone activation by CoFCM was proposed from the results of the electron paramagnetic resonance (EPR) and radical scavenger experiments.

研究领域: 环境科学 · 材料科学
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Scientific Reports · 2024 ·Vol. 14 ·期 1 ·1-10 · IF 3.8

Preparation of Ti3C2Tx modified rare earth doped PbO2 electrodes for efficient removal of sulfamethoxazole

Zhu Dancheng,Wu Yifan,Zheng Kai,Xu Hao,Chen Chao,Qiao Jun,Shen Chao

In this study, we deposited Ti 3 C 2 T x -modified, rare-earth-doped PbO 2 on the surface of a carbon fabric via electrodeposition. The surface morphology and electronic structure of the electrode were characterized with SEM, XRD and XPS. The layered Ti 3 C 2 T x did not change the structure of β-PbO 2 , and at the same time, it improved the crystallinity of the material and reduced the grains of PbO 2 . Electrochemical experiments showed that the addition of Ti 3 C 2 T x increased the electrochemical activity of the electrode and produced more H 2 O 2 , which contributed to the degradation of pollutants. The efficiency of sulfamethoxazole (SMX) degradation reached 95% after 120 min at pH 3 with a current density of 50 mA/cm 2 . Moreover, the electrode has good cycling performance, and the degradation efficiency was still 80% after 120 min after 10 cycles of recycling. Based on the intermediates identified by HPLC‒MS, a mechanism for SMX degradation was proposed. Our results will provide a new idea for the development of efficient electrocatalytic degradation of antibiotics.

CAS / MDL: 156-87-6 1306-38-3
研究领域: 环境科学 · 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Surface-bound sulfate radical-dominated degradation of sulfamethoxazole in the CuFeAl-LDH/peroxymonosulfate system: The abundant hydroxyl groups enhancing efficiency mechanism

Qing Xin,Siqi Liu,Shixu Lu,Zhenyu Chen,Pengzhan Han,Shuaishuai Xin,Qianwen Wang,Guocheng Liu,Chengzhi Zhou,Yanjun Xin,Qinghua Yan

In this study, a fast and efficient Cu 2 Fe 0.5 Al 0.5 -LDH/PMS water purification system was constructed to degrade sulfamethoxazole (SMX). The optimized Cu 2 Fe 0.5 Al 0.5 -LDH/PMS reaction system degraded 50% SMX for only 0.5 min, and 98.25% SMX for 10 min. The advanced characterization techniques proved that the abundant hydroxyl groups of Cu 2 Fe 0.5 Al 0.5 -LDH can form ≡M−(O)OSO 3 − complexes with PMS, resulting in reactive oxygen species (ROS) and promoting SMX degradation. Moreover, the electron transfer between the active bimetallic components played a synergistic role in the generation of ROS species. Compared with the electron transfer degradation mechanism, ROS mechanism contributed more to SMX degradation, in which surface-bound SO 4 − was the dominated active species. The possible degradation pathway and intermediate toxicity of SMX were proposed. This work provided a strategy to fully explore the catalytic degradation mechanism of heterogeneous catalysts in wastewater purification.

研究领域: 环境科学 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Synergistic multiple active species for the degradation of sulfamethoxazole by peroxymonosulfate in the presence of CuO@FeOx@Fe0

Yongli He,Jiali Zhang,Hongyu Zhou,Gang Yao,Bo Lai

In this study, bimetallic particles (CuO@FeO x @Fe 0 ) were prepared by displacement plating and calcination to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX). First, the key preparation parameters (i.e., theoretical Cu mass loading (TML Cu ) and calcination temperature) of CuO@FeO x @Fe 0 preparation were investigated by single-factor experiments. Then the properties of CuO@FeO x @Fe 0 were analyzed by scanning electron microscope energy dispersive spectrometry (SEM-EDS), energy dispersive spectrometry mapping (EDS-mapping), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Subsequently, effects of PMS dosage, CuO@FeO x @Fe 0 dosage and initial pH on the degradation of sulfamethoxazole were studied respectively. Meanwhile, the results of control experiments indicated that the initial SMX degradation efficiency of CuO@FeO x @Fe 0 system was slower, but the final degradation rate was higher than that of Fe 0 /PMS system, which was due to the sustained release effect of Fe 2+ . In addition, the quantitative experiment of SO 4 − indicated that SO 4 − generated continuously in CuO@FeO x @Fe 0 /PMS system. Furthermore, the detection results of quenching tests and electron paramagnetic resonance (EPR) revealed the generation of multiple reactive oxygen species (i.e., SO 4 − , HO , O 2 − , 1 O 2 ) in CuO@FeO x @Fe 0 /PMS system, which degraded SMX synergistically. Finally, the SMX degradation pathways were proposed based on the intermediates detected by Liquid Chromatography-Quadrupole time of flight – Mass Spectrum (LC-QTOF-MS/MS) and the activation mechanism of CuO@FeO x @Fe 0 /PMS system was analyzed in detail. This study provided a new insight on the application of CuO@FeO x @Fe 0 on organic pollutant degradation.

研究领域: 环境科学 · 化学工程
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

Simultaneous degradation of SMX for efficient nitrogen fixation to ammonia and hydrogen evolution using AgVO3@rGO-Ag3PO4 (110) heterojunction

Xueyu Wei,Saraschandra Naraginti,Xiaofan Yang,Xiaoping Xu,Jiyuan Li,Meiqing Zhu,Pengli Chen,Pei Jiang

The simultaneous degradation of organic pollutants and generation of value-added compounds like ammonia and hydrogen energy has recently gained considerable attention in photocatalysis . The present study deals with successful preparation of novel AgVO 3 nanowire@rGO-tetrahedral Ag 3 PO 4 (110) (AGA) heterojunction and utilized for enhanced generation of NH 3 and H 2 from N-containing antibiotic sulfamethoxazole (SMX) under visible light. The prepared catalyst was well characterized by XRD , SEM, TEM and XPS to confirm the formation of heterojunction . The results indicated that the composite exhibited 546.0 μmol g −1 of hydrogen evolution rate, which is approximately 3.6 (153.6 μmol g −1 ) and 5.1 (108.7 μmol g −1 ) times higher than the pure AgVO 3 and Ag 3 PO 4 respectively after 6 h. Similarly, 38.3 mg L −1 g −1 of NH 3 generation was observed during 6 h of SMX degradation, which is about 1.9 and 2.8 times higher than the pure AgVO 3 (20.1 mg L −1 g −1 ) and Ag 3 PO 4 (13.7 mg L −1 g −1 ) respectively. The formation of heterojunction between AgVO 3 and Ag 3 PO 4 not only promotes the transfer of electron but also prevents the recombination which eventually enhances the catalytic conversion of N-element to NH 3 and for H 2 generation during water splitting. Furthermore, the plausible degradation pathway in SMX was proposed and the results revealed that the SMX was mineralized by the composite further converted to NH 3 and generates H 2 during the degradation process . Thus, our study provides new insights into novel photocatalytic treatment methodologies for simultaneous degradation of SMX to produce NH 3 and H 2 as value-added compounds from antibiotic wastewaters during water treatment process.

研究领域: 环境科学 · 材料科学
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Journal of Water Process Engineering · 2024 · IF 6.3

Enhanced sulfamethoxazole degradation in aqueous media using a synergistic system with dielectric barrier discharge plasma, biochar-enriched iron concentrate, and persulfate

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.

CAS / MDL: 723-46-6
研究领域: 环境科学 · 化学工程
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MATERIALS RESEARCH BULLETIN · 2020 · IF 4.019

Fabrication of wool ball-like F-doped BiOCl0.4Br0.3I0.3 composite for effective sulfamethazine photocatalytic degradation

Ying Li,Jiahao Lai,Xiaoni Zheng,Siying Lv,Jing Yang,Shihai Cui

Novel material wool ball-like F-doped BiOCl 0.4 Br 0.3 I 0.3 has been successfully fabricated via a facile solvothermal method. In this work, the as-synthesized catalyst was characterized to examine the structure, morphology, optical and electrochemical properties. The catalyst was used in sulfamethazine degradation under visible-light irradiation. The optimized photocatalyst F-BiOCl 0.4 Br 0.3 I 0.3 (Bi:F = 3:2) exhibits superior activity and the degradation efficiency can reach 99.6 % in pH 6 within 60 min. There are two reasons to explain it: (i) The F-BiOCl 0.4 Br 0.3 I 0.3 has narrow band gap; (ii) Wool ball-like morphology can cause multiple reflections of the irradiated light, and availably prolong the action time. The primary oxidative species are holes and superoxide radicals. The possible degradation mechanism was discussed based on the experimental results.

CAS / MDL: 57-68-1
研究领域: 材料科学 · 环境科学
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Journal of Water Process Engineering · 2025 · IF 6.7

A “honeycomb” heterostructured α-MnO2 nanowire/NiCo2O4 hollow nanocages with superior photoelectrocatalytic performance for water purification

Yuejie Li,Yan Chen,Xinyue Wang,Khalil Md Ibrahim,Guowen Wang,Xinxin Zhang,Hongchao Ma

Recently, employing photoelectrocatalysis (PEC) strategy to eliminate environmental impact and hazards of hard-to-handle antibiotics such as sulfamethoxazole (SMX) has been given increasing attention. Herein, a “honeycomb” heterostructured α-MnO 2 nanowire/NiCo 2 O 4 hollow nanocages PEC catalyst is fabricated by using a continuous assembly process as following: (1) construction of α-MnO 2 nanowire carrier, (2) surface adhesion of ZIF-67, and (3) Co/Ni ion exchange. The as-synthesized Ti/α-MnO₂@NiCo₂O₄ demonstrated excellent PEC performance for degrading SMX, as compared with that of α-MnO 2 , α-MnO 2 @ZIF-67. Especially, the optimized Ti/α-MnO₂@NiCo₂O₄-30 showed removal rate of 98.2 % for SMX in 30 min, outstanding durability (~8000 s), and tolerable reusability (the removal rate can still reach 76.5 % for SMX after five cycles). The improvement of PEC performance for Ti/α-MnO₂@NiCo₂O₄ can be attributed to that the unique porous structure formed numerous electrochemically active sites, and the α-MnO₂ nanowire as common channel for charge transfer promoted the migration of induced carriers. The DFT calculation indicated that a II-scheme heterojunction can be formed over the α-MnO 2 @NiCo 2 O 4 composite, which can effectively inhibit the recombination of induced carriers, facilitate the degradation process. This work provides a valuable approach for constructing nanohybrids with targeted functionalities, opening new possibilities for the application of nanomaterials in wastewater treatment.

研究领域: 环境科学 · 纳米材料科学 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

High efficient activation of peroxymonosulfate by Co9S8 anchored in N, S, O co-doped carbon composite for degradation of sulfamethoxazole: Effect of sulfur precursor and sulfur doping content

Shizong Wang,Jianlong Wang

Cobalt sulfides as persulfate activator have received increasing interest in the field of persulfate-based advanced oxidation process. In this study, Co 9 S 8 anchored in N, S, O heteroatoms co-doped carbon (CoSx@N-S-O-C) composite was prepared with different sulfur precursors (sulfur, thiourea, thiophene and benzyl disulfide), and used to activate peroxymonosulfate (PMS) for sulfamethoxazole (SMX) degradation. The effect of temperature, pH, inorganic ions, humic acids and water components on SMX degradation was investigated. The results showed that sulfur precursor could regulate the catalytic activity of the composite through changing the cobalt speciation and carbon structure. The catalytic activity was highest when the molar ratio of sulfur to cobalt was 5:1 (CoS x @N-S-O-C-5). Sulfate radicals (dominant) and hydroxyl radicals contributed to SMX degradation. The intermediate products during SMX degradation were identified, and the possible pathway of SMX degradation was proposed. Pyridinic N, Co-N, cobalt, S 2− , S 2 2− , C-S-C and C-SO x were active sites for PMS activation.

研究领域: 环境科学 · 化学工程
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