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JOURNAL OF MATERIALS SCIENCE · 2020 ·Vol. 55 ·期 25 ·11609-11621 · IF 3.553

Biofilm eradication by in situ generation of reactive chlorine species on nano-CuO surfaces

Wang Wei,Peng Rui,Liu Jiali,Wang Zhenzhen,Guo Tao,Liang Qisheng,Carrier Andrew J.,Wang Li,Zhang Xu

Herein, we constructed a nano-CuO film on copper foil for the in situ generation of reactive chlorine species (RCS) for the contact killing of bacteria and biofilm suppression and dispersal. Both Staphylococcus aureus and Escherichia coli were susceptible to this treatment . Additionally, we demonstrate the solid nano-CuO interface-based heterogeneous Fenton chemistry rather than leached copper-ion-based homogeneous Fenton chemistry is responsible for RCS generation and bacterial cytotoxicity. This process is modulated by the H 2 O 2 and Cl − concentrations in bacterial growth environment. The potential applications for in situ generation of RCS might be the incorporation of CuO nanoparticles into functional food contact surfaces as well as coating materials for marine biofouling control.

研究领域: 微生物学 · 材料科学 · 环境科学
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TRANSACTIONS OF TIANJIN UNIVERSITY · 2018 ·Vol. 24 ·期 4 ·361-369 · IF 0

Fe–Mn/MCM-41: Preparation, Characterization, and Catalytic Activity for Methyl Orange in the Process of Heterogeneous Fenton Reaction

Zhang Xubin,Dong Jianxin,Hao Zhencheng,Cai Wangfeng,Wang Fumin

Active Fe- and Mn-loaded MCM-41 (Fe–Mn/MCM-41), which was synthesized via a hydrothermal reaction followed by impregnation, is used in the heterogeneous Fenton reaction to degrade methyl orange (MO) in aqueous solution. The synthesized samples were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N 2 adsorption–desorption isotherm analysis, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. Compared with Fe/MCM-41 and Mn/MCM-41, Fe–Mn/MCM-41 showed higher activity for MO degradation and mineralization. Effects of various operating parameters, such as pH, Mn content, and H 2 O 2 dosage, on the degradation process were subsequently investigated. Results of experiments on the effect of radical scavengers revealed that the degradation of MO could be attributed to oxidation by HO·. The synergy of Fe and Mn species in the Fenton oxidation process was also explained.

CAS / MDL: 7722-84-1 78-10-4
研究领域: 环境科学 · 催化材料 · 水处理技术
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2020 ·Vol. 27 ·期 11 ·12017-12029 · IF 3.056

Remediation of organic arsenic contaminants with heterogeneous Fenton process mediated by SiO2-coated nano zero-valent iron

Lv Yuancai,Huang Siyi,Huang Guofu,Liu Yifan,Yang Guifang,Lin Chunxiang,Xiao Gao,Wang Yonghao,Liu Minghua

Given their considerable solubility in water and potentially high toxicity to human health, organoarsenic compounds have become an emerging contaminant. Herein, a heterogeneous Fenton process mediated by SiO 2 -coated nano zero-valent iron (SiO 2 -nZVI) was employed to simultaneously remove the p -arsanilic acid ( p -ASA, a typical organoarsenic compound) and the released arsenic. The initial pH value significantly influenced on the degradation of p -ASA and at the optimal pH (3.0), p -ASA (10 mg L −1 ) could be completely oxidized to As(V), NH 4 + , and plentiful phenolic compounds such as phenol and p -hydroquinone via the cleavage of C–N and C–As bonds within 60 min in pure water. Meanwhile, although the formed lepidocrocite and magnetite on the surface of SiO 2 -nZVI significantly limited the reutilization, they played a vital role in the adsorption of the released As(V) and the residual arsenic levels in the effluent were as low as 0.031 mg L −1 , meeting both the drinking water standard of the World Health Organization (WHO) and the surface water standard of China (0.05 mg L −1 ). Furthermore, high-level dissolved organic matters (DOM) (> 2 mg C L −1 ) exhibited strong interference with both the oxidation of p -ASA and adsorption of arsenic, but the interference could be eliminated by increasing the SiO 2 -nZVI dosage or adding H 2 O 2 . Importantly, this system could completely remediate p -ASA in a short time and simultaneously avoid the secondary pollution caused by inorganic arsenic, which was significant for the remediation of organoarsenic pollutants in swine wastewater.

研究领域: 环境科学 · 化学工程
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ACS Applied Nano Materials · 2018 · IF 0

Preparation of Ultrasmall Goethite Nanorods and Their Application as Heterogeneous Fenton Reaction Catalysts in the Degradation of Azo Dyes

Zhengxin Liu,Lujie Zhang,Feihong Dong,Jie Dang,Kaile Wang,Dong Wu,Jue Zhang,Jing Fang

The discharge of azo dyes causes great harm to humans and the environment. Azo dyes can be degraded by a heterogeneous Fenton reaction catalyzed by α-FeOOH nanorods. However, because of the large size of conventional goethite nanorods, the reaction rate of the heterogeneous Fenton reaction is limited. In this study, we proposed a template method strategy for synthesizing ultrasmall α-FeOOH nanorods (SFNs) and investigated their use for catalyzing the degradation of an azo dye, methyl orange (MO). Transmission electron microscopy results suggested that the sizes of SFNs are much smaller than those of conventional nanorods (LFNs), and the catalytic efficiency of SFNs is 7.4 times higher than that of LFNs. This can be explained by the higher specific surface area and more catalytic sites of the catalyst. The degradation rate of MO increases with an increase in the concentrations of hydrogen peroxide (H2O2) and SFNs. Moreover, the MO degradation rate can reach 98% under the appropriate parameters after 60 min of reaction. In addition, reuse experimental results suggest that SFNs manufactured using our proposed approach achieved satisfied reusability, indicating that SFNs have potential application prospects in the degradation of azo dyes by catalyzing the heterogeneous Fenton reaction.

研究领域: 环境科学 · 材料科学
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Smart Materials and Structures · 2022 ·Vol. 32 ·期 2 ·025003 · IF 4.131

Study on heterogeneous Fenton reaction parameters for polishing single-crystal SiC using magnetorheological elastomers polishing pads

Da Hu,Huilong Li,Jiabin Lu,Qiusheng Yan,Qiang Xiong,Zhanliang Huang,Fenglin Zhang

Magnetorheological elastomers (MRE) are intelligent controllable materials used as polishing pads in chemical mechanical polishing (CMP), and the magnetic particles in the MRE polishing pad are used as solid-phase catalysts for heterogeneous Fenton reactions for oxidizing single-crystal SiC surfaces, thereby helping reduce the processing difficulty and obtain high-quality surfaces. The influence of the solid-phase catalyst (Fe3O4 mass fraction, particle size) and polishing solution environment (H2O2 concentration, pH value) on the CMP heterogeneous Fenton reaction polishing single-crystal SiC were investigated. The material removal behavior of the MRE polishing pad was investigated. The results demonstrated that the solid-phase catalyst, Fe3O4, has a better superior effect than the carbonyl iron powder (CIP). The polishing material removal rate (MRR) increased and the surface roughness (Ra) decreased with an increase in the Fe3O4 mass fraction. Superior polishing results were obtained at a particle size of 0.3 μm. The higher the H2O2 concentration in the polishing solution, the greater the MRR, with lower Ra at 10% concentration. The highest MRR and lowest Ra were achieved at pH = 3 in acidic environments. During polishing, the heterogeneous Fenton reaction can significantly enhance the removal ability of polishing materials. The MRR increased by 33.4% with the heterogeneous Fenton reaction compared with those without the heterogeneous Fenton reaction, and the contribution of the heterogeneous Fenton reaction to total material removal was 25.03%. The analysis of the SiC–Abrasive–MRE polishing pad contact state revealed that the heterogeneous Fenton reaction can oxidize the SiC surface and reduce the surface hardness, increasing the indentation depth δwa of the abrasive grain into the SiC surface and exhibiting greater material removal.

研究领域: 材料科学 · 化学机械抛光 · 智能材料
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Efficient oxidative degradation of fluconazole by a heterogeneous Fenton process with Cu-V bimetallic catalysts

Nuanqin Zhang,Chengjie Xue,Kuang Wang,Zhanqiang Fang

In this study, a novel Cu-V bimetallic catalyst (CuVOx) with abundant surface defects was successfully synthesized by hydrothermal method. Degradation experiment of emerging pollutant fluconazole confirmed that CuVOx exhibited higher catalytic activity, wider pH applicability and more satisfactory reusability than monometallic copper compounds. Electron paramagnetic resonance and radical quenching tests indicated that surface hydroxyl groups play a crucial role in the degradation of contaminants. By the introduction of vanadium into copper-based materials, several surface properties that are closely related to the reactivity of the copper catalysts such as adsorption capacity, surface defects, and active sites concentration were improved. It was also found that the electron-rich center around Cu/V active sites and surface oxygen vacancies are responsible for the rapid dissociation of H 2 O 2 and the efficient catalytic oxidation of fluconazole in CuVOx Fenton system. We also applied CuVOx Fenton to the degradation of various refractory organic pollutants, further confirming its excellent removal and detoxification efficiency for organic pollutants in the aquatic environment.

CAS / MDL: 144-55-8 136-32-3
研究领域: 环境科学 · 催化化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

Electrochemical sensor for a photoassisted heterogeneous Fenton self-oxidation signal amplification strategy

Wenjun Li,Yue Yang,Chaoyun Ma,Yiju Song,Xiuwen Qiao,Chenglin Hong

Traditional electrochemical immunosensors have stagnated due to the lack of signal tags and single signal amplification strategies. In this work, we propose a new signal amplification strategy, a photoassisted heterogeneous Fenton self-oxidation reaction, for the detection of prostate-specific antigen (PSA). A prepared ferric tetroxide (Fe 3 O 4 )@Carbon(C)@Glucose oxidase (GOD) heterogeneous Fenton electrochemical sensor is first immersed in a solution containing glucose, persulfate (S 2 O 8 2− ) and tannic acid (TA), and then it is irradiated with ultraviolet light at 365 nm. Utilizing a coupling reaction, S 2 O 8 2- promotes the use of ultraviolet light by Fe 3 O 4 @C−COOH@GOD to generate more OH radicals; furthermore, the coordination of tannic acid to Fe 2+ promotes the oxidation of Fe 2+ in Fe 3 O 4 to Fe 3+ by OH. This achieves a signal amplification of 3 times the value of the original system. More importantly, the Fenton reagent undergoes a self-oxidation reaction without the need to add a signal tag. The proposed immunosensor uses a new signal amplification strategy that can be used for detecting tumor markers. Additionally, due to the self-oxidation of the Fenton reagent and the C coating, the problem of signal tag leakage is effectively solved. The electrochemical immunosensor detects different concentrations of PSA and exhibits excellent analytical performance, with a detection limit of 0.17 pg/mL and a detection range of 0.5 pg/mL to 40 ng/mL. The prepared immunosensor provides a feasible method for the detection of cancer tumor markers.

研究领域: 生物医学工程 · 分析化学
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POWDER TECHNOLOGY · 2021 · IF 5.134

Degradation of methylene blue by a heterogeneous Fenton reaction catalyzed by FeCo2O4-N-C nanocomposites derived by ZIFs

Ting Zhang,Qingqing Ma,Mengqi Zhou,Changyu Li,Jianchao Sun,Weijie Shi,Shiyun Ai

Rationally designing efficient nanomaterials for heterogeneous activation of peroxymonosulfate (PMS) is necessary for environmental remediation. Nitrogen-containing carbon/FeCo 2 O 4 composites (FeCo 2 O 4 -N-C) were prepared by annealing the iron and cobalt in the ZIF-67 (Fe-Co-ZIF) precursor at different reaction temperatures. In the presence of PMS, 400 °C calcined nitrogen-containing carbon/FeCo 2 O 4 composites (FeCo 2 O 4 -N-C-400) was used as catalyst for heterogeneous Fenton degradation of methylene blue (MB) and nearly 100% MB was removed within 10 min without pH adjustment. FeCo 2 O 4 -N-C-400 had excellent catalytic activity profiting from the uniform distribution of bimetals and nitrogen doping, which ensured the exposure of sites with high catalytic activity. Free radical quenching experiments showed that a large number of reactive oxygen species (SO 4 .- and . OH) were the cause of pollutant degradation. At the same time, the possible degradation mechanism of MB in FeCo 2 O 4 -N-C-400/PMS system was proposed. In addition, FeCo 2 O 4 -N-C-400 can still degrade 60% of MB after four cycles, which indicated that the catalyst had long-term catalytic durability and recyclability.

研究领域: 环境科学 · 材料科学
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KEY ENGINEERING MATERIALS · 2022 · IF 0

Dewatering Treatment and Catalytic Application of Sludge by Glow Discharge Plasma

Ting Li,Shao Yong Huang,Jia Ming Gan,Min Li Shao,Lei Wang

In this paper, glow discharge plasma (GDP) was used to remove organic contaminants of sludge and improve sludge dewaterability. Fe-rich sludge as a catalyst combined GDP to form heterogeneous Fenton reaction, which was used to remove 2,4-dichlorophenoxyacetic acid (2,4-D) in aqueous solution. The surface micrographs and chemical composition of Fe-rich sludge was analysed by the Scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS). The effect of initial pH0 on hydrogen peroxide (H2O2) yield in GDP was discussed. The removal of 2,4-D was associated with the synergetic effect of adsorption and oxidative, and hydroxyl radicals (•OH) play a dominant role. This study provides an environmentally-friendly technology to improve sludge dewaterability and a potentially low-cost catalyst for 2,4-D removal in water, which is significant for the reuse of Fe-rich sludge.

研究领域: 环境科学 · 污水处理 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Investigation of the degradation and dehalogenation properties of florfenicol by heterogeneous Fenton reaction activated with MIL-53(Al)-supported nano zero-valent iron

Zhe Zhao,Wuming Xie,Zijun Huang,Haiming Cai,Yuemeng Ji,Baocong Zhao

The antibiotic florfenicol (FF) discharged into the aquatic environment may cause serious water pollution. Therefore, an effective way to eliminate FF antibiotics from the water bodies should be proposed. Herein, MIL-53(Al)-supported nano zero-valent iron (NZVI@MIL-53(Al)) was synthesized and applied to activate hydrogen peroxide (H 2 O 2 ) to spark the Fenton reaction for FF antibiotics removal. The characterization results demonstrated the successful loading and good dispersion of NZVI onto MIL-53(Al). 100 % FF antibiotics degradation could be achieved under the optimal reaction conditions, including an initial FF antibiotics concentration of 20 mg L −1 , initial solution pH of 3.0, NZVI@MIL-53(Al) dose of 25 mg L −1 , and H 2 O 2 concentration of 0.2 mM. And after four cycles, the FF antibiotic degradation efficiency was still 81.18 %. The lowest tolerance for HCO 3 − was observed while the degradation activity was maintained at the presence of Cl − and HA. EPR measurement and free radical quenching experiment showed that ·OH was the main reactive specie in the NZVI@MIL-53(Al)/H 2 O 2 system. FF antibiotics degradation involved hydroxylation reactions (electrophilic substitution), dehalogenation, hydrolysis, and cleavage based on the UPLC-MS/MS analysis and DFT calculation. Noteworthy, 0.247 mg L −1 of F − and 1.2 mg L −1 of Cl − were detected in the solution after the reaction due to the breakage of the stable C–Cl bond and C–F bond. Finally, this work revealed that the NZVI@MIL-53(Al), with high stability and recyclability, could be a potential heterogeneous catalyst for treating antibiotic wastewater.

研究领域: 环境科学 · 化学工程 · 材料科学 · 分析化学
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