Environmental Science-Nano
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2021
·Vol. 8
·期 12
·3629-3642
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IF 8.131
Jiaojiao Wang,Xiaoqing Jia,Denghui Shang,Liangbo Xie,Yi Li,He Zhang,Sihui Zhan,Wenping Hu
The long-term overuse of ciprofloxacin has resulted in its ubiquitous release into aquatic environments, seriously threatening public and ecological security. Herein, a photo-assisted-electro-Fenton-like (PAEF-like) system using p–n type Cu2O/Bi2MoO6 (CBM) as photoelectric catalyst was designed for efficient ciprofloxacin removal. The realization of photo-assisted function benefited from the perfectly constructed p–n heterojunction, which effectively regulated the carrier migration behaviors and drove the directional delivery of photoinduced electrons with flexible reactivity. Furthermore, photoinduced electrons directly or indirectly promoted the activation of H2O2 to enhance the ability of the PAEF-like synergy system to form ˙OH, improving the photoelectric catalytic activity. As dominant active species, ˙OH cooperated with h+ and ˙O2−, leading to the efficient elimination of ciprofloxacin. Finally, the degradation rate within 120 min reached almost 100%, and the corresponding kinetic constant was 208 and 1.5 times that of the photocatalytic and EF-like system, separately. Importantly, CBM-25% still maintained superior removal effect after four consecutive runs, revealing the high stability and practical feasibility of the PAEF-like system.
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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催化
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产品关联
DOI
高影响因子
CHEMOSPHERE
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2020
·
IF 5.778
Wei Wang,Yanchun Li,Yawei Li,Minghua Zhou,Omotayo A. Arotiba
A novel superhydrophobic gas diffusion electrode based on carbon black (CB)- polytetrafluoroethylene (PTFE) modified graphite felt cathode was prepared to increase oxygen mass transfer efficiency and produce hydrogen peroxide at the gas-liquid-solid three-phase interface without aeration. The gas diffusion electrode system was further tested for the degradation of sulfamethazine (SMT) by electro-Fenton (EF) and photoelectro-Fenton (PEF). In the EF process, SMT was removed effectively, but the mineralization degree was not high due to the generation of organic acids which were difficult to be further degraded. While in the PEF process, organic contaminant can be destroyed by the combined action of Fe 2+ /H 2 O 2 , UV/H 2 O 2 and UV radiation, and more efficient mineralization (>83.5%) at low current (50 mA) was attained, which might be attributed to the high H 2 O 2 utilization (70–90%), rapid regeneration of Fe 2+ and photolysis of intermediates. In addition, it was verified that the PEF system had a good adaptability to pH and pollutant concentration . Compared with aeration system, the use of this active gas diffusion cathode in electrochemical advanced oxidation processes significantly reduced energy consumption.
研究领域:
环境科学
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化学工程
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污水处理
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产品关联
DOI
PubMed
高影响因子
Frontiers in Environmental Science
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2022
·
IF 5.411
Ma Yameng,Huang Xiao,Han Qi,Yu Jianghua,Yu Fengjiao,Zhu Jia
The strong stability of Cu–ethylenediaminetetraacetic acid (Cu–EDTA) results in the low decomplexation efficiency by the traditional Fenton process. For breaking this limitation, a three-dimensional electro-Fenton (3D-EF) system was constructed to study the decomplexation of Cu–EDTA at different pH, and the effects of Fe2+ concentration, particle electrode dosage, current density, and coexisting ions on decomplexation performance were investigated. The results showed that 3D-EF exhibited high pollutant removal efficiency in a wide pH range compared with the traditional electro-Fenton process. The optimal conditions for the removal of Cu–EDTA were as follows: the pH was 7, Fe2+ was 1 mmol L−1, granular activated carbon was 2 g L−1, and current density was 10 mA cm−2, and the optimum Cu–EDTA removal efficiency reached 90.95%. In addition, the presence of Cl− slightly improved the decomplexation efficiency, whereas NO3− and HPO42− inhibited the removal of Cu–EDTA. The kinetics of Cu–EDTA decomplexation in all experimental groups followed the first-order kinetic equation.
研究领域:
环境工程
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化学工程
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水处理
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DOI
高影响因子
Water
·
2022
·Vol. 14
·期 9
·1420
·
IF 3.53
Juan Peng,Yameng Ma,Xiao Huang,Jianghua Yu,Fengjiao Yu,Jingsi Gao
Ni-ethylenediaminetetraacetic acid (Ni-EDTA) poses serious threats to the ecological environment and human health, due to its acute toxicity and low biodegradability. The decomplexation efficiency of Ni-EDTA through the conventional Fenton process has been constrained to pH; thus, other appropriate approaches are required to destroy the stable chelate structure at a neutral pH. In this study, the effect of operating parameters such as the pH, Fe2+concentration, particle electrode dosage, current density, and coexisting ions was studied. The results revealed that the 3D-EF system owned advantages for the removal of Ni-EDTA in the broadening of the pH application window. The Ni-EDTA removal efficiency in the 3D-EF system reached 84.89% after 120 min at a pH of 7. In addition, the presence of coexisting ions slightly affected the decomplexation efficiency of Ni-EDTA.Keywords:Ni-EDTA;three-dimensional electro-Fenton;neutral pH;decomplexation
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Yusi Tian,Minghua Zhou,Yuwei Pan,Xuedong Du,Qi Wang
Molybdenum sulfide (MoS 2 ) was for the first time used as a co-catalyst to enhance the performance of Fe 0 based heterogeneous electro-Fenton (Fe 0 -EF) process for the degradation of sulfamethazine (SMT), which was belonging to the sulfonamide family and extensively used as growth promoters and antibacterial drugs. Compared with Fe 0 -EF process, MoS 2 /Fe 0 -EF process could enhance the rate constant of SMT degradation 2 times under the optimal conditions of current 50 mA, MoS 2 dosage 0.02 g L -1 , Fe 0 dosage 0.224 g L -1 , and initial pH 4, in which SMT could be completely degraded within 10 min while 42% TOC could be achieved after 60 min reaction. The role of MoS 2 as co-catalyst in MoS 2 /Fe 0 -EF process and Fe 2+ /Fe 3+ cycle was supported by iron elemental analysis, transmission election microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) characterizations. Owing to the characteristics of co-catalysis, MoS 2 could greatly facilitate the Fe 3+ /Fe 2+ recycle reaction by the exposed Mo 4+ active sites, which significantly promoted the decomposition of H 2 O 2 that generated in Fe 0 -EF system and improved the generation of hydroxyl radical. Besides, a possible degradation pathway of SMT was proposed and the stability of MoS 2 /Fe 0 -EF process for SMT removal and TOC mineralization was certified base on five consecutive runs. The real wastewater test and energy consumption and economic analysis confirmed its advantage and cost-effectiveness for application. In all, this study provides a new perspective for improving heterogeneous Fe 0 -EF process with MoS 2 for highly efficient and rapid degradation of antibiotics.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Lele Cui,Zhiwen Li,Qingqing Li,Meifei Chen,Wenheng Jing,Xuehong Gu
The development of transition metal oxide-based integrated carbonaceous materials for use as bifunctional electrodes of high stability and activity in the heterogeneous electro-Fenton (EF) process is supposed to have great potential in environmental governance. Herein, Cu/CuFe 2 O 4 (CCFO) with different Cu 0 ratios were synthesized by a facile one-step solvothermal approach. These materials were subsequently used to fabricate modified graphite felt through the polytetrafluoroethylene (PTFE)-bonding technique. Importantly, with its hydrophobicity PTFE effectively inhibited metal leaching from the thus obtained cathodes and improved the oxygen utilization rate. Cathode performance in EF-based tetracycline (TC) degradation was found to increase with Cu 0 ratio. The observed increase in activity was attributed to Cu 0 enhancing the 2-electron oxygen reduction reaction selectivity (i.e., H 2 O 2 production) and endowing the cathode with abundant electron-rich centers that accelerated active Fe(II) regeneration, causing rapid conversion of H 2 O 2 to hydroxyl radical ( OH). The possible TC mineralization pathway was inferred by liquid chromatography–mass spectrometry (LC–MS) analysis, and a catalytic mechanism of the heterogeneous EF process was proposed. The most effective cathode fabricated displayed high stability even at pH 3 (0.84 ± 0.11 mg/L Fe and 1.35 ± 0.17 mg/L Cu leaching) and exhibited nearly 80% TC removal efficiency after five oxidation cycles, demonstrating its potential use in heterogeneous EF technology for efficient and durable wastewater treatment.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2013
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IF 5.257
Peng Liao,Songhu Yuan,Mingjie Chen,Man Tong,Wenjing Xie,Peng Zhang
A novel Pd-based electro-Fenton (E-Fenton) process has recently been developed to transform organic contaminants in groundwater. However, it only produces H2O2 and requires addition of Fe2+. In this study, an innovative approach is developed to effectively regulate the generation of Fe2+ from an iron cathode in a three-electrode system in addition to H2O2 production. The Fe2+ is then used for the Pd-catalytic transformation of methyl tert-butyl ether (MTBE) in groundwater. Results from batch experiments suggest Fe2+ accumulation follows pseudo-first-order kinetics with rate quantitatively regulated by current and pH, and MTBE can be completely transformed. In a specially configured three-electrode column using iron as the first cathode, the localized acidic conditions develop automatically in the iron cathode and Pd zone by partitioning the current between the two cathodes, leading to controllable generation of Fe2+ and H2O2. Effects of electrolyte concentrations and types as well as humic acid on MTBE transformation are slight. The stable transformation (∼70%) in a long-term study (20 days) suggests this improved Pd-based E-Fenton process is sustainable to produce Fe2+, H2O2, and appropriate pH conditions simultaneously for transforming organic contaminants. This study presents a new concept of generating Fe2+ from an iron cathode for the processes requiring Fe2+.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CLAY SCIENCE
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2023
·
IF 5.6
Ting Zhang,Ge Bai,Nan Cai,Yongqian Lei,Pengran Guo,Jingwei Xu
Since the outbreak of COVID-19, the extensive use of epidemic control drugs such as Arbidol (ARB) and Acyclovir (ACV) has significantly increased and the environmental pollution caused by these residues has attracted increasing attention. In this article, a novel montmorillonite graphene-like carbon hybrid Fe 3 O 4 compound (Mt/GH/Fe 3 O 4 ) as particle electrode catalyst was prepared and applied in three-dimensional-electro-Fenton (3D-EF) for the ARB and ACV degradation. The structure and composition of the compound catalyst were characterized. The degradation efficiency of targets was significantly increased in the 3D-EF degradation system and even more thorough for the degradation of targets, compared with simple 2D, 3D, and EF catalytic degradation systems. The degradation rate of antiviral drugs can reach >90% in 5 min with excellent stability. The research demonstrated that the clay mineral with a special structure loaded with graphene-like carbon and Fe 3 O 4 had supplied an ideal reaction medium for the electro-Fenton reaction. Mt./GH/Fe 3 O 4 -based 3D-EF degradation system would have promising applications in the degradation and removal of antiviral drug residuals in the environment.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Water
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2020
·
IF 0
Mingyue Zhao,Zhicheng Cui,Liang Fu,Fabrice Ndayisenga,Dandan Zhou
The slow reduction of Fe(III) to Fe(II) in electro-Fenton technology limits pollutant removal and causes Fe sludge production. This study hypothesizes that Shewanella, a dissimilatory iron-reducing bacteria, can accelerate the iron reduction of the Fenton reaction. A Shewanella biofilm coupled with Fe2O3 coated electrode (F/S) was used to drive the electro-Fenton reaction, and compared the results with the singlet Fe2O3 (F) anode and Shewanella biofilm anode (S). Meanwhile, dissolved oxygen (DO) is studied as an important influencing factor. The suitable DO was verified at ∼2 mg/L, phenol removal of F/S was 67% higher than that of the sum of three other singlet systems. The chemical oxygen demand (COD) removal was 72% and 50% higher than that of F and S, respectively. F/S corrosion current (Icorr) was 6.3 times higher than F, and induced hematite to transform into Fe2PO5 and FeOOH on the anode. Long-term operation showed that phenol was almost 100% removed for F/S; COD removal was generally 20% higher than F; thus, the toxicity of the effluent could be significantly decreased. The total Fe loss did not exceed 10% at the end of operation. This paper provides a feasibly novel method for electro-Fenton reaction, by employing Fe-reducing bacteria.
研究领域:
环境科学
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微生物学
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产品关联
DOI
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Xueyue Mi,Yi Li,Xingming Ning,Jinhu Jia,Haitao Wang,Yuguo Xia,Yan Sun,Sihui Zhan
The emergence of antibiotics in the environment, especially in drinking water, poses potential harm to human health. It’s urgent to develop effective methods to remove antibiotics in drinking water. In this work, a series of mesoporous Mn x Co 3−x O 4 nanoparticles with high surface area were successfully synthesized and firstly used as effective stable electro-Fenton catalysts to degrade ciprofloxacin (CIP). The removal of CIP achieved to 100% within 5 h. Experimental and density functional theory (DFT) studies verified the existence of redox pairs of Mn 2+ /Mn 3+ and Co 2+ /Co 3+ . Scanning electrochemical microscopy (SECM) results suggested that the redox reaction capacity of MnCo 2 O 4 was enhanced and the electron transfer rate on the surface of this bimetallic oxide was 2.67 and 1.6 times the number of MnO 2 and Co 3 O 4 , respectively. The effective degradation of CIP was mainly associated with the increased electron transfer rate and advanced redox reactivity owing to the synergistic effect of manganese and cobalt entrapped in the matrix of mesoporous structure which provided more accessible active sites. The degradation intermediates and possible process mechanism were investigated in detail. The reusability of MnCo 2 O 4 -CF cathode was evaluated five cycles with minimal ion leaching which the concentration of Mn and Co in the system was lower than 2.5 and 3.4 ppm, respectively. This work provides further understanding for removal process of organic pollutants by investigation of redox couple and electron transfer rate of the promising MnCo 2 O 4 -CF cathode.
研究领域:
环境科学
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材料科学
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生物学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2023
·
IF 4.5
Jingjing Zhan,Min Zhan,Xiujuan Zhang,Yiwen Zhang,Tianxiang Wang,Yang Liu,Shoukai Wang
There are many reports related to the hollow carbon nanosphere with the applications in electrochemistry. However, it remains insufficient research in the field of electro-Fenton. In this study, we discovered that hollow carbon spheres can be obtained by the self-assembly of β-cyclodextrin in one step, without using any templates and toxic organic solvents. Meanwhile, activation methods were explored to create more pores and regulate the surface groups in the outer shell of the materials, which are key factors affecting the H 2 O 2 production capability. It is found that H 2 carbonization effectively converts a large number of sp 2 -C bonds on the surface of the materials to sp 3 -C, providing more active sites for reaction during the electrocatalytic process. The results show that the hollow carbon nanosphere after dual activations has the most H 2 O 2 production rate at 70 mg·L -1 ·h −1 , higher than those of carbon solid spheres and unmodified hollow carbon nanospheres. In the application of electro-Fenton, this material exhibits the degradation efficiency of 95.5 % for 50 mg·L -1 p -nitrophenol, fully meeting the needs of environmental remediation. The whole preparation and activation process is simple, environmentally friendly, easy to be scaled up and has broad application prospects. This paper enhanced the understanding of common hollow carbon spheres in the hot research field of electro-Fenton.
研究领域:
环境科学
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材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Li Lin,Fangjie Zhang,Xing Hou,Linlin Wang,Weijie Wu,Longfei Wang,Yi Li,Haijiao Xie
The advanced oxidation processes based on the electro-Fenton reactions show great potentials as a wastewater treatment approach for removing emerging contaminants. In the electro-Fenton system, some factors still exist affecting the treatment efficiency, e.g., the formation of iron sludge, a narrow pH working range, and slow conversion rates between Fe 2+ and Fe 3+ . In this research, a novel heterogeneous flow-through electro-Fenton system was constructed, and carbon felt was used as the template material for the preparation of an etched carbon felt cathode loaded with zero-valent iron and iron oxide (Fe@Fe 2 O 3 /ECF) for the degradation of bisphenol A , which addressed the aforementioned issues. The Fe@Fe 2 O 3 /ECF electrode showed excellent performance across a pH range between 3 and 11, with exceptional stability and resistance to other substances in water. For the three pollutants, bisphenol A, tetracycline and ciprofloxacin, the highest degradation efficiency can reach 99.3 %. Compared to traditional electro-Fenton systems, the novel process exhibited superior performances due to synergistic effects from feasible flow design, enhanced electrochemical reactivity and greater exposure of active sites. Through electron spin resonance and free-radical quenching experiments, it was determined that the primary species participating in the heterogeneous electro-Fenton process were the hydroxyl radical and superoxide anion. Specifically, the hydroxyl radical was identified as playing a pivotal role in the degradation of bisphenol A. After a continuous operation of 240 min, the electrode showed low metal ion leaching rate and good stability, with the concentrations of leached Fe and Co ions to be only 17 and 7 μg/L, respectively. Meanwhile, the removal efficiency was only decreased by 5.7 % during the process. Through density functional theory calculation and intermediate product analysis, three potential degradation pathways were proposed, with the cleavage of carbon bonds serving as the main degradation approach. The toxicity analysis demonstrated that the intermediates were generally less toxic than BPA during treatments. This research provides a fresh means for promoting a valence state cycling of ferric species in electro-Fenton system, which has potential applications in wastewater treatment containing emerging contaminants.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）