Catalysis Science & Technology
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2021
·Vol. 11
·期 11
·3715-3723
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IF 6.119
Daoqing Liu,Qianwei Li,Jinbao Hou,Huazhang Zhao
The coexistence of aliovalent cations may facilitate the formation of electronic and ionic defects, altering the catalytic properties of manganese oxide. In this paper, a series of mixed-valent manganese oxides (MnOx) were prepared by a hydrothermal route and tested for heterogeneous activation of peroxydisulfate for Orange II degradation in aqueous solution. The morphology, crystal structure and surface chemistry of the MnOx were adjusted by the addition of ethanol in the hydrothermal process. The physicochemical properties were characterized and evidence from X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) indicated that MnOx exhibited a mixed crystal phase structure of Mn2O3, Mn3O4 and MnO2. The catalytic properties of the three samples prepared with 5%, 10%, and 20% volume fractions of ethanol (denoted as MnOx-5, MnOx-10, and MnOx-20) were found to be related to the valent states of Mn, and MnOx-10 exhibited a better performance with a mole ratio of Mn4+/ Mn2+ close to 1.0. The electrochemical characterization demonstrated that MnOx-10 performed a more effective redox process which may determine the catalytic activity of MnOx. Moreover, quenching tests, electron paramagnetic resonance (EPR) and gas chromatography-mass spectrometry (GC-MS) were used to evaluate the possible activation processes of peroxydisulfate (PDS) and the intermediates of Orange II degradation. This catalyst preparation strategy provides a new idea for the preparation of high-efficiency environmental catalysts.
研究领域:
环境科学
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催化化学
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材料科学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 14
·6664-6676
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IF 8.867
Zepei Bao,Lin Ye,Beibei Fang,Lijun Zhao
Herein, Fe0.32Co0.68 binary metal nanoparticles synthesized at room-temperature were loaded onto a novel hierarchical flower-like γ-Al2O3@C composite, which improved the stability and dispersity of the Fe0.32Co0.68 nanoparticles. The freshly prepared Fe0.32Co0.68/γ-Al2O3@C displayed good adsorption of Orange II (100 mg L−1, 973.55 mg g−1). Subsequently, the used Fe0.32Co0.68/γ-Al2O3@C adsorbent (Fe–Co oxide/γ-Al2O3@C) was reused as a peroxymonosulfate (PMS) catalyst. Amazing results were obtained, which demonstrated that Fe–Co oxide/γ-Al2O3@C can highly efficiently decompose Orange II (60 mg L−1, 1 min; 90 mg L−1, 2 min, 120 mg L−1, 7 min and 150 mg L−1, 10 min) as a PMS catalyst. It also exhibited good general degradation of different organic pollutants and excellent reusability (98%, tenth cycle) due to the structural stabilities of γ-Al2O3@C. Further, an experiment was carried out to treat high concentrations of Orange II (200 mg L−1) with the Fe0.32Co0.68/γ-Al2O3@C nanocomposite. After adsorption, PMS was added, and 98% degradation occurred within 5 minutes. The combination of adsorption and PMS advanced oxidation techniques may be one of the effective ways to deal with high-concentration dye wastewater.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Water
·
2024
·Vol. 16
·期 21
·3109
·
IF 3
Zheng Zhang,Libin Zhao,Jingyuan Tian,Shaojie Ren,Wei Zhang
Persulfate-based advanced oxidation processes have emerged as a promising approach for the degradation of organic pollutants in aqueous environments due to their ability to generate sulfate radicals (SO4−·) within catalytic systems. In this study, peroxydisulfate (PDS) and peroxymonosulfate (PMS) were investigated with the natural vanadium–titanium magnetite (VTM) as the activator for the degradation of acid orange II. The degradation efficiency increased with higher dosages of VTM or persulfate (both PDS and PMS) at lower concentrations (below 10 mM). However, excessive PMS (higher than 10 mM) in the PMS/VTM system led to the self-consumption of free radicals, significantly inhibiting the degradation of acid orange II. The VTM-activated PDS or PMS maintained an effective degradation of acid orange II in a wide pH range (3~11), suggesting remarkable pH stability. The SO4−·was the main active species in the PDS/VTM system, while hydroxyl radical (·OH) also contributed significantly to the PMS/VTM system. In addition, PMS exhibited better thermal stability during VTM activation. Coexisting ions in an aqueous environment such as bicarbonate (HCO3–), carbonate (CO32–), and hydrogen phosphate (HPO42–) had obvious effects on persulfate activation. Our study systematically investigated the different activation processes and influencing factors associated with PDS and PMS when the natural VTM was used as a catalyst, thereby providing new insights into the persulfate-mediated degradation of organic pollutants in aqueous environments.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
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2021
·
IF 4.094
Xiaorui Zhang,Yu Mei,Hao Cheng,Jianfeng Ma,Fang Zhu,Sridhar Komarneni
NiO and CeO 2 composite metal oxides (NiO–CeO 2 ) were synthesized by sol-gel method to investigate a degradation system by persulfate (PS) activation with the assistance of visible light (Vis). The phase composition of NiO–CeO 2 was detected by X-ray diffraction (XRD), the morphology of NiO–CeO 2 was characterized by scanning electron microscope (SEM), and the result of X-ray photoelectron spectroscopy (XPS) proved the element composition and valence state of the NiO–CeO 2 . In the Vis/PS/NiO–CeO 2 system, the degradation rate of Orange II using a concentration of 50 mg/L was as high as 90% in 15 min but it increased to as high as 99% in 60 min. Mechanism studies have shown that the combination of NiO and CeO 2 generated more oxygen vacancies , and activated persulfate to generate active oxygen species. Moreover, the effects of visible light , persulfate concentration and pH were evaluated, and the results showed that the participation of visible light and persulfate could significantly increase the degradation efficiency of Orange II, but pH had little effect on the degradation. Quenching experiments and detection by ESR showed that O 2 ‾, •SO 4 ‾, •OH, and 1 O 2 all contribute to the removal of Orange II. In addition, the recovery and reuse properties of NiO–CeO 2 may lead to sustainable treatment of wastewater.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2016
·Vol. 92
·期 7
·1601-1612
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IF 2.738
Jiahua Lu,Qing Liu,Zhongduo Xiong,Zhijun Xu,Yingjie Cai,Qiang Wang
BACKGROUND Synthetic dyes are present in the wastewater from many industrial processes and they cause serious problems to human and aquatic life. The development of a novel and effective peroxymonosulfate (PMS) activator is proposed to eliminate dyes pollution. A new magnetic nanocomposite, Fe 3 O 4 @C/MnCo 2 O 4 , was prepared and characterized. The activity of Fe 3 O 4 @C/MnCo 2 O 4 as heterogeneous catalyst for PMS activation was evaluated by the decolorization of Acid Orange II (AO II). RESULTS With a ‘Fe 3 O 4 @C/MnCo 2 O 4 + PMS’ system, the dye solution could be nearly completely decolorized in about 25 min over a wide pH range (pH 4.1−8.1), and 98% removal could be achieved in 15 min without pH adjustment (pH = 6.38). The influence of solution pH, dosage of catalyst and PMS, reaction temperature, and PMS activation mechanism were studied. It was found that sulfate radicals were the primary species responsible for the oxidation of AO II. The catalyst was magnetically separable and displayed good stability and reusability, giving six cycles of use without deterioration in its performance. CONCLUSION This study demonstrated the simple recycling and high activity of Fe 3 O 4 @C/MnCo 2 O 4 composite in PMS activation for the decolorization of AO II solution. It provides a promising way for the decontamination of organic pollutants. © 2016 Society of Chemical Industry
研究领域:
环境科学
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化学工程
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高影响因子
Journal of Environmental Sciences
·
2019
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IF 3.556
Shanshan Su,Yuyang Liu,Wei He,Xianchun Tang,Wei Jin,Yaping Zhao
Persulfate activation has been applied as one of the efficient advanced oxidation processes (AOPs) to remediate polluted environments. In this study, a novel α-FeOOH anchored by graphene oxide (GO)-carbon nanotubes (CNTs) aerogel (α-FeOOH@GCA) nanocomposite activated persulfate system (α-FeOOH@GCA + K 2 S 2 O 8 ) was applied for decolorization of Orange II (OII). The decolorization of OII was remarkably enhanced to a level of ~ 99% in this system compared with that of pristine α-FeOOH (~ 44%) or GO-CNTs (~ 18%). The enhanced catalytic activity of α-FeOOH@GCA was due to the formation of a heterojunction by α-FeOOH and GO-CNTs as confirmed by the presence of Fe–O–C chemical bonds. The degradation intermediates of OII were comprehensively identified. The proposed degradation pathway of OII begins with the destruction of the conjugated structures of OII by the dominant reactive oxygen species , surface-bound SO 4 •− . The decolorization efficiency of OII by the α-FeOOH@GCA activated persulfate system decreased from the first to third cycle of recycling. Ultraviolet (UV) irradiation or introduction of a small amount of Fe 2+ could restore the activation of this system. The results show that the α-FeOOH@GCA persulfate activation system promises to be a highly efficient environmental remediation method for organic pollutants .
研究领域:
环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2018
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IF 5.091
Zhibo Yang,Liang Zhu,Lin Chen
Core-shell structured NH 2 -functionalized UiO-66 magnetic composites (γ-Fe 2 O 3 @C@UiO-66-NH 2 ) were fabricated via a simple, facile and green approach to investigate their adsorption behaviors towards different organic dyes (methylene blue, malachite green , acid fuchsin and acid orange II). Different characterization methods containing XRD , TEM , EDXA , FTIR, BET and XPS were used to indicate that the as-prepared γ-Fe 2 O 3 @C@UiO-66-NH 2 material exhibited core-shell structure and excellent surface performance. Adsorption experiments showed that γ-Fe 2 O 3 @C@UiO-66-NH 2 could selectively adsorb anionic dyes and effectively separate the mixture, which might be mainly ascribed to the negatively-charged anionic dyes as opposite to the positively-charged Zr metal sites in γ-Fe 2 O 3 @C@UiO-66-NH 2 . The kinetics and adsorption isotherm of acid orange II and acid fuchsin adsorption in γ-Fe 2 O 3 @C@UiO-66-NH 2 were also investigated. For acid orange II and acid fuchsin, the maximum adsorption capacity obtained from the Langmuir isotherm model was 48.12 mg/g and 31.54 mg/g, respectively. Moreover, γ-Fe 2 O 3 @C@UiO-66-NH 2 exhibited good structural stability and reusability, which suggesting that γ-Fe 2 O 3 @C@ UiO-66-NH 2 as an easy-prepared adsorbent material exhibited great application potential in the selective removal of dyes from water systems.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2017
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IF 4.217
Chaoqun Tan,Yujie Dong,Lei Shi,Qin Chen,Shengwei Yang,Xiaoyu Liu,Jinfeng Ling,Xuefeng He,Dafang Fu
The degradation of Orange II (Org II) by ferrous activated peroxymonosulfate (PMS) was inspected. The maximum degradation efficiency of 62.3% in 90 min occurred at 0.286 mM [PMS] 0 , corresponding to 1:1 molar ratio of Fe 2+ : PMS. Results show that poor recovery of Fe 2+ accounts for poor degradation in the slow stage. The species of reactive radicals were determined through indirect way by quenching agents, as well as directly by in situ EPR spin trapping tests. Results indicated that hydroxyl radicals instead of sulfate radicals were responsible for Org II degradation. The removal of Org II degradation would increase to 93.3% in 90 min as reaction temperature increased to 60 °C. The activation energy for PMS and Fe 2+ /PMS alone was calculated to be 77.2 kJ/mol and 34.7 kJ/mol, respectively. The removal efficiency of total organic carbon (TOC) was 11.0% and 43.8% when [Fe 2+ ] 0 :[PMS] 0 :[Org II] 0 was 5:5:1 and 34:34:1, respectively. The main degradation products of Org II in system were supposed to be heterocyclic compounds containing a five-atom ring. Results demonstrated that Fe 2+ /PMS technology is promising technology for water pollution.
研究领域:
环境科学
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化学工程
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2015
·Vol. 27
·期 1
·1020-1030
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IF 1.569
Zhou X. J.,Shi P. H.,Qin Y. F.,Fan J. C.,Min Y. L.,Yao W. F.
Co 3 O 4 /graphene composites were synthesized and their high catalytic activity for the activation of peroxymonosulfate to remove the azo dye (Orange II) in aqueous solutions was found. As for the poor quality of rGO by the chemical process of graphene oxide, here, pristine graphite was exfoliated into graphene flakes through direct sonication with assistance of cetyltrimethyl ammonium bromide, which serves as a dispersant in the solvothermal procedure. The physical and chemical performance of Co 3 O 4 /graphene was characterised by X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy and thermogravimetric analysis. The obtained Co 3 O 4 nanocrystals were 15–25 nm in size and connected with each other to form the shape of sticks dispersing on graphene sheets. The Co 3 O 4 /graphene composites completely degraded Orange II solutions within 10 min, the catalyst can be reutilized, and the catalytic activity of the Co 3 O 4 /graphene dropped slightly after four successive runs. In addition, the mechanism for the formation of Co 3 O 4 /graphene nanostructures is also illustrated.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2020
·Vol. 14
·期 6
·956-966
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IF 3.552
Ni Qingzhuo,Cheng Hao,Ma Jianfeng,Kong Yong,Komarneni Sridhar
A ZnMn 2 O 4 catalyst has been synthesized via a sucrose-aided combustion method and characterized by various analytical techniques. It is composed of numerous nanoparticles (15–110 nm) assembled into a porous structure with a specific surface area (SSA) of 19.1 m 2 ·g −1 . Its catalytic activity has been investigated for the degradation of orange II dye using three different systems, i.e., the photocatalysis system with visible light, the chemocatalysis system with bisulfite, and the photochemical catalysis system with both visible light and bisulfite. The last system exhibits the maximum degradation efficiency of 90%, much higher than the photocatalysis system (15%) and the chemocatalysis system (67%). The recycling experiments indicate that the ZnMn 2 O 4 catalyst has high stability and reusability and is thus a green and eximious catalyst. Furthermore, the potential degradation mechanisms applicable to the three systems are discussed with relevant theoretical analysis and scavenging experiments for radicals. The active species such as Mn(III), O 2 •− , h + , e aq − , SO 4 •− and HO • are proposed to be responsible for the excellent degradation results in the photo-chemical catalysis system with the ZnMn 2 O 4 catalyst.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
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2023
·
IF 4.1
Wei Sun,Qing Xu,Qili Liu,Tianliang Wang,Zhaixin Liu
Efficient magnetic solid phase extraction using covalent organic frameworks (COFs) can find important applications in food safety. In this work, a sulfonate-functionalized magnetic COF (Fe 3 O 4 @COF-SO 3 Na) was synthesized by self-polycondensation of two-in-one monomer 1,6-bis(4-formylphenyl)-3,8-bis((4-aminophenyl) ethynyl)) pyrene (BFBAEPy) on the surface of aminated Fe 3 O 4 and a thiol-yne click reaction. It was further adopted as an adsorbent for the efficient magnetic solid-phase extraction (MSPE) of basic orange II. The selective adsorption experiment indicated that it displayed selective adsorption ability to basic orange II due to the ion exchange, hydrogen bonds, and π-π interactions. Under the optimized conditions, the proposed MSPE method coupled with HPLC-DAD showed excellent linearity in the range of 0.05–0.5 µg/mL (R 2 = 0.9997) for basic orange II. The lower limits of detection (LODs) for basic orange II were 1.0–1.4 µg/L for three food samples: yellow croaker, paprika and dried bean curd. The recoveries were 90.1–98.8% with relative standard deviations (RSDs) below 4.2%. Therefore, this work provides an effective strategy to modify magnetic COFs as absorbents in MSPE. Due to the tunability of functional groups in thiol‑yne click reactions, the functional groups of magnetic COFs can be readily designed to enrich their multifunctional applications. Meanwhile, this work proposed a new method to detect trace amounts of basic orange II in food samples.
研究领域:
分析化学
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食品安全
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产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2024
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IF 3.3
Dongao Xie,Changxin Tang,Dan Li,Jiren Yuan,Feigao Xu
FeOCl has attracted much attention for its good photo-Fenton properties. However, there are still some limitations to the removal efficiency of organic pollutants. Visible-light-responsive FeOCl/CdS quantum dot composites were prepared by calcination to overcome their flaws, and their catalytic activity was explored by the degradation of acid orange II (AO-II). The experimental results showed that the FeOCl/CdS composites exhibited better catalytic performance than pure components. The F1Cd0.5 composite (mass ratio of FeOCl to CdS is 1:0.5) achieved 98.5% removal efficiency of AO-II, which is 14.8 times higher than that of FeOCl+CdS under similar experimental conditions; moreover, the F1Cd0.5 composite still exhibits a high stability after five cycles. According to the characterization and experimental results with density functional theory calculations together, it is proposed that the type II carrier transfer-separation mechanism plays a leading role in enhancing the photodegradation performance of the photo-Fenton catalysts. This study provides a new idea to further improve the catalytic efficiency of the photo-Fenton technology for organic pollutant degradation.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）