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ENVIRONMENTAL TECHNOLOGY · 2022 · IF 3.475

Degradation of COD in antibiotic wastewater by a combination process of electrochemistry, hydroxyl-functionalized ball-milled zero-valent iron/Fe3O4 and Oxone

Chun-Feng Wang,Yue-Yi Li,Ai-Hong Li,Nan Yang,Xiao-Wen Wang,Yin-Ming Li,Ye Zhang

In this study, the significant iron-based material, hydroxyl-functionalized ball-milled zero-valent iron/Fe3O4 (HFB-ZVI/Fe3O4) was employed for the experiments. The performance of the Electro + HFB-ZVI/Fe3O4 + Oxone system for the degradation of chemical oxygen demand (COD) in antibiotic wastewater was investigated. A direct current was applied between a graphite plate anode and two iron plate cathodes, and a series of operational parameters, such as applied electric current, the dosage of HFB-ZVI/Fe3O4 composite, the dosage of Oxone, and initial solution pH, were explored to evaluate the oxidation process. The application of electric current enhanced the gradual degradation of COD and the increase of current intensity accelerated COD degradation. The neutral condition was favourable for the rapid degradation of COD in a short reaction time by the Electro + HFB-ZVI/Fe3O4 + Oxone process and promoted the degradation efficiency of COD. An increase of electric current gradually decreased the reaction solution pH, the larger the electric current applied in the reaction process, the lower the final pH of the reaction solution. Under the optimal experimental conditions (1 g/L HFB-ZVI/Fe3O4 composite, 0.3 g/L Oxone, current intensity = 500 mA, initial solution pH = 7.85), Electro + HFB-ZVI/Fe3O4 + Oxone achieved 99% COD degradation in antibiotic wastewater. Radicals quenching experiments indicated the contribution to COD degradation by hydroxyl radicals (HO•), sulphate radicals (SO4•–) and other oxidants were 66.03%, 24.014% and 9.756%, respectively. The possible mechanism of COD degradation in the Electro + HFB-ZVI/Fe3O4 + Oxone system was also discussed in this study. The findings in this work provided useful information for the treatment of wastewater.

CAS / MDL: 1317-61-9
研究领域: 环境科学 · 水处理工程 · 化学工程
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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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CHEMICAL ENGINEERING JOURNAL · 2011 · IF 3.074

Performance of CuO/Oxone system: Heterogeneous catalytic oxidation of phenol at ambient conditions

Fei Ji,Chaolin Li,Lei Deng

CuO particles were synthesized by a hydrothermal method and used to activate Oxone for advanced oxidation of phenol in aqueous solution. The effects of several parameters on the degradation efficiency of the process were investigated. The as-prepared catalyst exhibited high activity in degradation of phenol and 100% decomposition and 86% TOC removal could be achieved in 60   min at the optimum conditions. Moreover, the catalyst was demonstrated to have good stability and reusability. Radical quenching studies were conducted to classify the type of active radicals present in the reaction and X-ray photoelectron spectroscopy (XPS) was applied to investigate the transformation of the chemical state of copper. According to the experimental results, a reasonable mechanism was proposed to interpret the catalytic process.

研究领域: 环境科学 · 催化化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2018 · IF 3.779

Degradation of Levofloxacin by heterogeneous activation of oxone using Co(OH)2/graphene composites

Yunqing Pi,Peng Zhao,Lingjia Ma,Yangdan Cao,Huiqing Gao,Shuying Dong,Jianhui Sun

The Co(OH) 2 /reduced graphene oxide hybrids (Co(OH) 2 /rGO) was prepared and used as catalyst to enhanced heterogeneous activation of Oxone for the decomposition of Levofloxacin (LVF). The Co(OH) 2 /rGO composites with different Co(OH) 2 loading have been successfully synthesized, where the sample contain 20% Co(OH) 2 exhibited superior activation, attributing to the synergistic effect between Co(OH) 2 and rGO. Meanwhile, the effects of some important reaction parameters on the decomposition of LVF by Co(OH) 2 /rGO/Oxone process were investigated. The results indicated that the decomposition rate of LVF(>94.5%) was increased with the increasing of Oxone concentration, and 20% Co(OH) 2 /rGO dosage neutral pH. Moreover, the Co(OH) 2 /rGO catalyst showed high activity and stability during the repeated experiments.

CAS / MDL: 7782-42-5
研究领域: 环境科学 · 材料科学 · 药学
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RSC Advances · 2016 ·Vol. 6 ·期 94 ·91791-91797 · IF 3.289

Different Co-based MOFs templated synthesis of Co3O4 nanoparticles to degrade RhB by activation of oxone

Jia-yi Pu,Jin-quan Wan,Yan Wang,Yong-wen Ma

In this study, Co-based MOF with a 2D structure, 3D microrod structure and 3D nano-dodecahedral structure was synthesized by the coordination of cobalt ions and different organic ligands. Then, Co3O4, which was derived from these Co-based MOFs, was used to activate oxone for RhB degradation. It was found that the morphology and structure of the templates can significantly influence the formation of the nano Co3O4 products, which has an indirect effect on the catalytic ability of the resulting Co3O4 for oxone to degrade RhB. Among the products, nano-sphere Co3O4, which was derived from a template with a 3D nano-dodecahedral structure (ZIF-67) can effectively activate oxone to degrade RhB. Under neutral conditions, the rate constant of the degradation of RhB (0.1 mM) was 0.0509 min−1 with 50 mg L−1 catalyst and 1.0 mM oxone based on first-order kinetics. In addition, the influence of a series of parameter factors (pH, the dosage of catalyst and oxone) on the catalyst was also studied. Low cobalt ion dissolution (0.04 mg L−1 at pH = 3, <0.01 mg L−1 at pH = 7) and good recyclability (degradation rate of RhB after 5 cycles: close to 96%, 89% at pH = 7, pH = 3) further proved that the as-prepared Co3O4 can be used as a promising catalyst.

研究领域: 环境化学 · 材料科学 · 催化化学 · 纳米技术 · 环境污染治理
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Catalysts · 2023 ·Vol. 13 ·期 2 ·410 · IF 3.9

Preparation of di-[EMIM]CoCl3 Ionic Liquid Catalyst and Coupling with Oxone for Desulfurization at Room Temperature

Shaokang Wang,Hang Xu

The intermediate di-[EMIM]Cl was synthesized from methyl imidazole and 1,4-dichlorobutane and then reacted with cobalt chloride at 105 °C to prepare a bi-[EMIM]CoCl3ionic liquid catalyst. The di-[EMIM]CoCl3catalyst coupled with oxone to remove sulfur-containing organics in octane. The di-[EMIM]CoCl3catalyst was characterized by HNMR, FTIR, TG, and SEM–EDS. The dibenzothiophene (DBT) was dissolved in octane to prepare a model oil with an initial sulfur content of 500 ppm. Six grams of the model oil was added. The results showed that the optimal dosages of di-[EMIM]CoCl3, oxone (20 wt%), and [BMIM]BF4extractant were 1 g, 2 g, and 2 g, respectively. At the optimum temperature of 45 °C, 100% of sulfur was removed after 40 min. After di-[EMIM]CoCl3was recycled five times, the sulfur removal percentage remained above 91%. The sulfur removal percentages for different sulfur-containing organics followed the order of dibenzothiophene (DBT) > benzothiophene (BT) > 4,6-dimethyldibenzothiophene (4,6-DMDBT). The oxidation product was determined to be DBTO2by GC–MS analysis, and the oxidation mechanism was discussed. The active oxygen atoms of oxone oxidized DBT to form DBTO, and then persulfate oxidized DBTO to DBTO2via an identical oxidation mechanism.Keywords:dicationic ionic liquids;cobalt chloride;oxone;desulfurization;catalytic oxidation

研究领域: 化学工程 · 环境科学
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FUEL · 2022 · IF 8.035

A fully-organic polymerization carrier calix[4]resorcinarene supported cobalt ionic liquid catalyst with oxone for desulfurization

Hang Xu,Shaokang Wang,Fengmin Wu,Qinlin Yuan,Yafei Guo,Yinke Zhang,Xuefeng Wei,Jun Zhang

One of the disadvantages of using inorganic solid catalysts is the formation of solid waste. The use of fully-organic solid catalysts can reduce secondary pollution by simple combustion or bio-degradation. Here, an organic polymerization carrier, calix[4]resorcinarene, with polyhydroxyl characteristics, was synthesized. A cobalt containing ionic liquid was successfully chemically bonded to the hydroxyl groups on the carrier surface using 3-chloropropyltrimethoxysilane as linking agent. The resulting fully-organic supported ionic liquid catalyst was coupled with oxone for desulfurization. The micro-structure of the catalyst was composed of a porous spatial network structure. The reaction system exhibited excellent dibenzothiophene (DBT) removal (93.3%) after 90 min under the optimum experimental conditions (20 °C, 6 g of model oil with an initial sulfur content of 1000 ppm, 0.2 g of 20 wt% oxone solution with a dosage frequency of three, 15% of CoCl 2 , 0.15 g of catalyst, and 2 g of [Bmim]BF 4 ). After six regeneration cycles, the sulfur removal remained above 90%. The desulfurization kinetics and mechanism were also discussed, and it was found that the hyperbolic model provided a better fit to the experimental data compared to the pseudo first-order model. The likely mechanism involves DBT being extracted using the ionic liquid [Bmim]BF 4 before being oxidized by the catalyst/oxone system to form DBTO 2 , which is easily removed from the system using polar solvents.

研究领域: 化学工程 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

S-doped TiO2 photocatalyst for visible LED mediated oxone activation: Kinetics and mechanism study for the photocatalytic degradation of pyrimethanil fungicide

Tao Li,Amal Abdelhaleem,Wei Chu,Shengyan Pu,Fei Qi,Jing Zou

The degradation of pyrimethanil (PYR) was investigated through the activation of oxone by the S-TiO 2 (ST) photocatalyst under visible LED irradiation. The catalyst characterization revealed that the sulfur doping mechanism was based on the cation (S 6+ ) substitution of Ti 4+ in TiO 2 lattice. The optimal molar ratio of S/Ti at 0.25 was proven efficient in the PYR degradation. Influences of various reaction parameters including ST loading, oxone dosage, PYR concentration, and initial solution pH were examined. SO 4 •- , • OH, 1 O 2 , O 2 •- , and h + were found to be the reactive species generated in the ST/Oxone/Vis LED process. Different natural water constituents exerted dissimilar effects because of the generation of additional reactive species or their radical scavenging capabilities. Moreover, the reusability test indicates the ST photocatalyst is reusable and stable. A series of degradation intermediates was detected via four major degradation pathways. Overall, the ST/Oxone/Vis LED process was demonstrated to be a promising approach for the removal of organic pollutants.

研究领域: 环境科学 · 催化化学
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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

Anchored highly stable Fe–Mn bimetallic catalyst in Al2O3 ceramic membranes for boosting Oxone activation and efficient degradation of emerging micropollutants

Zhenkai Wang,Yifan Li,Yanfang Su,Sheng-Peng Sun,Xiaoning Wang,Zhangxiong Wu,Winston Duo Wu,Xiao Dong Chen

Catalytic membrane integrating membrane filtration and advanced oxidation in one single-step is promising in addressing emerging micropollutants issue in water, the challenges in catalytic activity and stability still limit their practical application. This study successfully anchored highly stable Fe–Mn bimetallic catalyst (FMBC) in Al 2 O 3 -based microfiltration and ultrafiltration ceramic membranes channel (named as FMBC@Al 2 O 3 -MF or UF) via a novel in situ fabrication strategy. Characterization results revealed that FMBC was anchored on the membrane channel wall of Al 2 O 3 -MF/UF, which enabled boosting Oxone activation to generate sulfate radical and hydroxyl radical at circumneutral pH (e.g., 7.0–9.0) and with great stability. Notably, FMBC@Al 2 O 3 -UF exhibited a remarkable activity and anti-interference capability in actual water matrices, which resulted in efficient degradation of emerging micropollutants such as carbamazepine, crotamiton, diethyltoluamide, gemfibrozil and ibuprofen in lake water and municipal wastewater treatment plant secondary effluent at environmentally relevant concentrations. Moreover, FMBC@Al 2 O 3 -MF/UF also displayed high cleaning efficiency toward natural organic matter (NOM) and effluent organic matter (EfOM) fouling via Oxone activation. Besides, the intermediates of carbamazepine degradation were identified, and most of them had decreased aquatic toxicity based on Ecological Structure Activity Relationship (ECOSAR) prediction. The high activity, stability and environmentally friendly property of the as-prepared FMBC@Al 2 O 3 -MF/UF make them promising application for advanced treatment of emerging micropollutants in water.

CAS / MDL: 3317-61-1 2403-88-5
研究领域: 环境科学 · 水处理技术
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Materials Research Express · 2022 ·Vol. 9 ·期 9 ·095504 · IF 2.025

Study on the synthesis and characterization of CoTiO3 catalysts and their catalytic properties in Oxone activation for the degradation of tetracycline antibiotic in water

Xiaohui Zhao,Hui Zhou,Qiong Hua,Chengyu Wang,Xiaodan Wang,Ke Zhang,Hongpei Zhang,Binguo Zheng,Junling Niu

The chemical degradation of sulfate by activated Oxyone has the advantages of high degradation capacity, wide pH range and convenient transportation and storage, making it one of the most attractive advanced oxidation processes (AOPs). Besides, Co is the metal most capable of activating Oxone to produce sulfate. Therefore, it is critical to develop Co-based catalyst, an effective and recyclable heterogeneous catalyst, for activating Oxone to degrade tetracycline. In this study, CoTiO3 was extensively investigated for the activation of Oxone to generate sulfate radicals and degrade tetracycline antibiotics. The results showed that more than 95% of tetracyclines could be degraded at the amount of CoTiO3 catalyst of 0.02 g, the Oxone reagent concentration of 0.4 mmol l−1, and the pH value of 7. The removal rate of tetracyclines could still reach more than 85% after the CoTiO3 composite was repeatedly used for four consecutive cycles. These results indicate that CoTiO3/Oxone can be explored as an effective system for degrading long-lived organic pollutants.

CAS / MDL: 60-54-8
研究领域: 环境科学 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Nonradical activation of Oxone over Fe-doped nitrogen carbon (Fe@NC) armor catalysts for efficient degradation of anthropogenic phenolics (p-nitrophenol, 4-chlorophenol) in groundwater matrices

Lei Su,Yifan Li,Zhenkai Wang,Yao-Yin Lou,Qi-Zheng Zheng,Zhangxiong Wu,Sheng-Peng Sun

Iron-based catalysts are widely used in peroxysulfate-based AOPs but suffering from low catalytic performance at neutral pH conditions, which limits the application in groundwater remediation. Herein, this study investigated the efficacy, mechanism and long-term durability of Fe-doped nitrogen carbon (Fe@NC) armor catalysts toward peroxysulfate activation for the degradation of anthropogenic phenolics (APs) in groundwater matrices. The results showed that nonradical activation of Oxone (i.e., HSO 5 – ) was obtained over the as-prepared Fe-3 % @NC-700 catalyst, high-valent Fe species ( Fe(IV) O) and 1 O 2 were identified as the dominant reactive species for the efficient degradation of APs by experiments and density functional theory (DFT) calculations. Notably, the DFT results indicated that HSO 5 – was favorably adsorbed on the Fe atoms owing to the electrostatic interaction, which transformed exothermically into SO 4 2– and 1 O 2 over Fe 3 C, accompanied by the generation of Fe(IV) O. Additionally, the Fe-3 % @NC-700 catalyst displayed long-term activity for in situ activation of Oxone in groundwater matrices without pH adjustment, resulting in ΔAPs: ΔOxone stoichiometry efficiencies at 4.2–5.0 % . Wheat seeds germination tests revealed that the biotoxicity of the treated water was reduced notably by the present catalytic system, which holds large potential application in treatment of APs-contaminated groundwater.

CAS / MDL: 141-78-6
研究领域: 环境科学 · 催化化学 · 地下水污染治理
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