JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Yubo Wu,Honglin Lin,Xuyun Gao,Zhiyan Liu,Yulun Nie
The Fe 3+ /Fe 2+ cycle has been identified as the rate-limiting step in the Fenton system, and many efforts have been made to promote the Fe 3+ reduction via external electrons provided by various electron donors. However, how to design an efficient electron transport pathway and then inhibit the invalid electron shuttle has been largely underestimated. In this study, two kinds of heterogeneous Fenton catalysts of CuO@Fe 2 O 3 and CuO@C@Fe 2 O 3 were prepared. The key role of carbon in transporting electrons as an electron bridge and its enhancement mechanism in photo-assisted Fenton-like performances were explored in detail. Compared with CuO@Fe 2 O 3 , the removal efficiency of tetracycline (TC) and the corresponding pseudo-first order reaction rate constants over CuO@C@Fe 2 O 3 increased significantly from 88.6 % and 0.1054 min −1 to 99.7 % and 0.2058 min −1 , respectively. Based on a series of probe experiments, visible light irradiation can promote the reduction of Cu 2+ to Cu + , then the carbon in CuO@C@Fe 2 O 3 can effectively transfer electrons from Cu + to Fe 3+ , enhancing the Fe 3+ /Fe 2+ cycle and the following Fenton-like efficiency. Since more ·OH while less ∙O 2 - was produced over CuO@C@Fe 2 O 3 , which further supports the fact that the enhanced Fe 3+ /Fe 2+ cycle was due to the transfer electron from Cu + to Fe 3+ instead of the Haber-Wiss mechanism. Hence, this study provides new insight for effectively improving the transfer efficiency and effective utilization of electrons in Fenton 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
CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Yiting Lv,Jinjuan Xue,Zhaoxia Chen,Jianan Qu,Kaiwen Huang,Mingxin Wang,Wei Sun
Photocatalytic production of H 2 O 2 has garnered significant attention, but the use of sacrificial reagents in H 2 O 2 photosynthesis and the subsequent limited H 2 O 2 activation efficiency would impede its practical application in water decontamination. In this work, hydrothermal carbonaceous carbon/NH 2 -MIL-101(Fe) (abbreviated as HTC-cf/NMIL-101(Fe)) heterojunction was fabricated through a solvothermal strategy, and serving as a self-sufficient photo-Fenton-like catalyst to in-situ generate and activate H 2 O 2 . Hydrothermal carbonaceous carbon derived from cost-effective waste coffee grounds, serving as a green and sustainable photocatalyst, demonstrated high H 2 O 2 production rate of 612 μmol/g/h without the need for sacrificial reagents or aeration assistance. Moreover, the excellent self-sufficient photo-Fenton activity for HTC-cf/NMIL-101(Fe) can be obtained, which ascribed to the synergistic effect of self-generated H 2 O 2 production as well as the in-situ catalytic H 2 O 2 decomposition of • OH by Fe species in NMIL-101(Fe) and photogenerated electrons. The optimized HTC-cf/NMIL-101(Fe) photocatalyst showed simultaneous improvements in both H 2 O 2 production and activation capabilities. Impressively, the effective circulation of Fe 3+ /Fe 2+ in NMIL-101(Fe), aided by photogenerated electrons, results in a 5-fold increase toward H 2 O 2 decomposition rate constant (K d ) compared to HTC-cf alone under light irradiation in open-air conditions. The enhanced charge separation and appropriate band structure of HTC-cf/NMIL-101(Fe) photocatalyst assured the high selectivity of two-electron O 2 -reduction to H 2 O 2 . HTC-cf/NMIL-101(Fe) displayed excellent photocatalytic sterilization efficiency against E. coli and S. aureus under visible light, and its sterilization application in actual water was also demonstrated. Notably, the adaptability of this system to ambient conditions, including open-air atmosphere, non-sacrificial reagents, and low leaching of Fe ions, highlights the promising practical utility of the HTC-cf/NMIL-101(Fe) photocatalyst.
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 COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Chengbo Bai,Yuhan Zhang,Qiong Liu,Chengxin Zhu,Jun Li,Rong Chen
To address the observed decrease in efficiency during Fe 2+ -mediated persulfate (PDS) activation caused by slow electron transfer rates and challenges in cycling between Fe 3+ /Fe 2+ states, we devised a strategy to establish interfacial complexation between Fe 3+ and Bi 2 MoO 6 in the presence of PDS. The proposed approach facilitates more efficient capture of photogenerated electrons, thereby accelerating the rate-limiting reduction process of the Fe 3+ /Fe 2+ cycle under visible light irradiation and promoting PDS activation. The Bi 2 MoO 6 /Fe 3+ /PDS/Vis system demonstrates complete degradation of organic pollutants, including Atrazine (ATZ), carbamazepine (CBZ), bisphenol A (BPA), and 2,4-dichlorophenol (DCP) at a concentration of 10 mg/L within a rapid reaction time of 30 min. Radical scavenging experiments and electron paramagnetic resonance spectra (EPR) confirm that the sulfate radical (•SO 4 − ) is the dominant species responsible for organic contaminant degradation. The real-time conversion process between Fe 3+ and Fe 2+ was monitored by observing changes in iron species forms and concentrations within the reaction system. X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy verify the formation of a complexation between Fe 3+ and Bi 2 MoO 6 , facilitating anchoring of Fe 3+ onto material surface. Based on these findings, we propose a reliable mechanism for the activation reaction. This work presents a promising heterogeneous PDS activation method based on Fe 3+ /Fe 2+ cycle for water treatment.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Xue Cui,Hongbin Yu,Yunhe Gong,Xinhong Wang,Ying Lu,Gang Zhang
A novel core-shell heterojunction photocatalyst Ta 3 N 5 @FeTaO 4 /Mn x O y was designed for efficient persulfate activation to enhance the photocatalytic performance. Ta 3 N 5 @FeTaO 4 /Mn x O y was synthesized using a two-step impregnation-calcination method, and tetracycline was selected as the model pollutant. The results indicated that the tetracycline degradation by Ta 3 N 5 @FeTaO 4 /Mn x O y was 3.79 and 13.42 times faster than those by Ta 3 N 5 @FeTaO 4 and Ta 3 N 5 , respectively. Pollutant degradation via radicals (·OH, SO 4 · − and O 2 · − ) and non-radicals (Fe(IV) and 1 O 2 ) was verified by probe tests, quenching experiments, and EPR analysis. The homologous growth heterojunction promoted the separation of charge carriers owing to the matched structure and seamless interface between Ta 3 N 5 and FeTaO 4 . The loaded Mn x O y enhanced persulfate adsorption and facilitated Fe 3+ /Fe 2+ cycling, consequently improving persulfate activation and the photocatalytic degradation of pollutants. This study reveals the often-overlooked role of iron-based catalysts to generate a wider range of reactive species, offering a new perspective to design Fenton-like photocatalytic materials.
研究领域:
环境科学
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催化材料
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产品关联
DOI
高影响因子
Journal of Cleaner Production
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2023
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IF 11.1
Yang Yang,Wenqing Zhen,Tingting Zhao,Maoquan Wu,Shouchun Ma,Liyan Zhao,Jie Wu,Li Liu,Jiaxu Zhang,Tongjie Yao
Fenton/photo-Fenton reaction was limited by slow Fe 3+ /Fe 2+ cycle, low H 2 O 2 activation efficiency, and narrow applicable pH range. Here, Fe atoms doped MoS 2 (Fe–MoS 2 ) with abundant of low-valence Mo δ+ (0 < δ < 4) was prepared. Benefiting from the powerful reduction capacity of Mo δ+ , the rate-limiting step of Fe 3+ reduction was significantly accelerated. Nearly 100% of H 2 O 2 utilization efficiency was realized. Importantly, 90% of H 2 O 2 was effectively activated to be • OH. As a result, tetracycline degradation rate in photo-Fenton reaction catalyzed by Fe–MoS 2 was 5.8 and 4.2 times higher than those of MoS 2 and Fe–MoS 2 -Hyd (prepared by hydrothermal reaction). In comparison with MoS 2 and Fe–MoS 2 -Hyd whose efficient work range were limited in acidic condition, Fe–MoS 2 was a pH-universal catalyst (pH = 2.6–14.0) by taking advantage of the exposed Mo δ+ and photoinduced electrons, largely improving the environmental tolerance. This work simultaneously addressed three bottlenecks in Fenton/photo-Fenton reaction, and provided a new strategy for the preparation of catalysts with powerful catalytic performance and high environmental adaptability.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Hongji Chen,Yan Wu,Huiping Xiao,Hongfei Yin,Qian Fei,Chunyu Yuan,Qiuyu Zhao,Yujin Zhang,Yongzheng Zhang,Woonming Lau
Owing to the low conversion efficiency of Fe 3+ to Fe 2+ during the peroxymonosulfate (PMS) activation process, the design of an efficient Fenton-like catalyst is still a challenge. In this work, 0D/2D Co-doped Fe 2 O 3 /g-C 3 N 4 (CNCFO) composite catalysts were constructed for organic pollutant degradation, where the Co-doping not only boosts the conversion efficiency of Fe 3+ to Fe 2+ , but also acts as active site for PMS activation. Among them, CNCFO2 showed excellent catalytic performance, where 96.4% of MO could be degraded within 45 s. X-ray photoelectron spectroscopy (XPS) confirmed that the cobalt doping promoted the cycle of Fe 3+ /Fe 2+ , which was responsible for the enhanced PMS activation. Meanwhile, the good stability and reusability of CNCFO2 itself provide opportunities for its potential practical applications. Based on systematical characterizations, the Z-scheme photo-Fenton mechanism was proposed. This study offers a fresh perspective on the advancement of designing highly efficient Fenton-like catalyst for applications in the field of environmental purification.
研究领域:
环境科学
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催化材料
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Caiwen Wu,Tianyi Guo,Yuhan Chen,Qiang Tian,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
Photoinduction is widely used to accelerate the Fe 3+ /Fe 2+ circulation in Fe 3+ /H 2 O 2 Fenton oxidation, however, the remained challenges in developing a facile, economical, and efficient synthetic methodology for the preparation of high-performance Fe-based Photo-Fenton catalyst and inevitably forming iron sludge limit its applications. Herein, starch-derived carbon (SC) encapsulated Fe 3 O 4 (Fe 3 O 4 @SC) magnetic nanocomposites are synthesized by mechanical activation treatment combined with high-temperature pyrolysis method using cassava starch as the carbon source. The photoelectrochemical properties of Fe 3 O 4 @SC are regulated by C O Fe bonds and oxygen vacancies in Fe 3 O 4 @SC, as well as graphitization of SC, which effectively accelerate the Fe 3+ /Fe 2+ circulation in Fe 3 O 4 @SC + H 2 O 2 system under visible light, thus Fe 3 O 4 @SC shows excellent catalytic performance and superior stability for the degradation of tetracycline hydrochloride, and the initiation rate constant is 2.4 times higher than that in dark. Moreover, quenching experiments and electron spin resonance results confirm that OH, O 2 − , and h + ( OH plays a critical role) are generated in the catalytic system of Fe 3 O 4 @SC + H 2 O 2 + visible light. This work provides new insights into a green and facile approach for the synthesis of Photo-Fenton catalysts, providing new avenue for the acceleration of Fe 3+ /Fe 2+ cycle under visible light-driven Fenton process.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Yun Ji,Zhelin Song,Yu Xu,Yanlin Zhang
In this work, typical refractory pollutant Rhodamine B (RhB) was effectively degraded by Cu-Fe LDHs/Bi 2 WO 6 composite in the photo-Fenton process. The hydrothermal synthesis of Cu-Fe LDHs/Bi 2 WO 6 composite with ethylene glycol as reductant created the multivalent coexistence of the same metal element to achieve a self-circle redox reaction between metals. The photo-Fenton process by Cu-Fe LDHs/Bi 2 WO 6 incredibly eliminated the limitation of strong acidic pH value applied in the Fenton process. ∙OH generated by Cu-Fe LDHs/Bi 2 WO 6 was 5 times that of Cu-Fe LDHs during the photo-Fenton process. The complete degradation of RhB in the photo-Fenton process under the optimal conditions of initial pH= 6, 5 mmol/L of H 2 O 2 , and 1 g/L of Cu-Fe LDHs/Bi 2 WO 6 dosage was far more than 46% of RhB degradation in the photocatalytic process and 76% of RhB degradation in the Fenton process. Cu-Fe LDHs/Bi 2 WO 6 composite exhibited the excellent redox ability, electron transfer ability and reusability during the photo-Fenton process. The acceleration of Fe 3+ /Fe 2+ cycles in the Cu-Fe LDHs/Bi 2 WO 6 /H 2 O 2 /Vis system was mainly ascribable to the combination of efficient transfer of photogenerated electrons and self-circle redox of Fe 3+ /Cu + . It is expected for the promising application of multivalent bimetallic photo-Fenton catalysts and rendering enlightenments for photo-Fenton catalytic oxidation reaction.
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
CATALYSIS LETTERS
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2025
·Vol. 155
·期 10
·1-13
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IF 2.4
Chen Shiqi,Huang Zhixuan,He Wentao,Wang Xinyu,Yang Zhiwei,Zhang Jing
Molybdenum nitride, because of the strong metal-support interaction between nitrogen and the metal, exhibits activity superior to that of bare metals, demonstrating its effectiveness as a co-catalyst to address the slow kinetics of the iron reduction in the Fenton process. Here, we introduced Mo 2 N as a co-catalyst to accelerate the cycles of Fe 3+ /Fe 2+ within a Fenton-like system consisting of Fe 3+ and H 2 O 2 , thereby enhancing the activation of hydrogen peroxide to generate reactive oxygen species (ROS). The system demonstrates excellent recyclability and stability. XPS spectroscopic analyses reveal that Mo(III) and Mo(IV) species on the Mo 2 N surface are capable of reducing free Fe(III), while FTIR analyses show nitrogen (N) and nitrogen oxide (NO x ) facilitate the adsorption and coordination of iron. Both homogeneous and heterogeneous reduced iron species are active in the activation of H 2 O 2 . EPR spectroscopy further confirms that the primary ROS generated are hydroxyl radicals (·OH) and superoxide anions (·O 2 − ). This study not only underscores the feasibility of Mo 2 N-based Fenton-like systems but also provides a new strategy for promoting the practical application of Fenton chemistry. Graphical
研究领域:
环境化学
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催化
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材料科学
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物理化学
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分析化学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Suzhou Xu,Can Liu,Xuping Jiang,Xinyu Wang,Shijin Zhang,Yanting Zhang,Qingguo Wang,Weiling Xiong,Jing Zhang
The performance and mechanisms of a titanium carbide (Ti 3 C 2 ) MXene modified Fe 3+ /hydrogen peroxide (H 2 O 2 ) system were compared in detail under dark and visible light conditions, with a new mechanism proposed for the reaction and reduction of MXene by Fe 3+ . Using Bisphenol A (BPA) as the target pollutant, the degradation of BPA by the Fe 3+ /H 2 O 2 system was improved after adding MXene in the dark, and the degradation rate of BPA was ≥ 95 % within 12.5 min under visible light, six times higher than that in the dark. Fe 2+ was ascertained to be the effective component responsible for H 2 O 2 activation to produce ·OH. SEM , XPS, ICP, XRD, and FTIR spectroscopy , analyses show that MXene and Fe 3+ form a complex, and then MXene reacts with Fe 3+ by breaking the Ti–C bonding to accelerate the Fe 3+ /Fe 2+ cycle. MXene uses photogenerated electrons to promote this reaction under visible light. In addition, quenching experiments and electron spin resonance spectroscopy results show that ·OH and O 2 •− are the main reactive oxygen species under visible light, while ·OH is the main active species in the dark. MXene thus effectively uses O 2 to form O 2 •− under visible light and promotes the Fe 3+ /Fe 2+ cycle. This study provides a theoretical basis for the combination of visible light catalysis and the advanced oxidation process of a Ti 3 C 2 MXene.
研究领域:
环境科学
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化学工程
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材料科学
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高级氧化过程
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2020
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IF 5.778
Fengxia Chen,Daojian Tang,Ya Wang,Tuo Li,Jiahai Ma
A novel catalyst which integrates heterogeneous and homogenous Fenton reactions is designed and fabricated by encapsulating 2,5-dihydroxy-1,4-benzoquinone (2,5-DBQ) in ECDP-Fe 3 O 4 , a composite of Fe 3 O 4 nanoparticles immobilized on a β-cyclodextrin polymer (ECDP) with ethylene diamine tetraacetic acid (EDTA) as cross-linking agent. The 2,5-DBQ@ECDP-Fe 3 O 4 has superior catalytic performance for 4-nitrophenol and 2,4-dichlorophenol degradation compared with control systems. Mechanism study revealed that although the initial active site is Fe 3 O 4 loaded on ECDP, the actually catalyst is the iron ions released from Fe 3 O 4 but confined within the composite. EDTA in β-cyclodextrin polymer can improve both the solubility and adsorption capacity to H 2 O 2 of Fe 3 O 4 . The quinone molecules 2,5-DBQ in the β-cyclodextrin cavity can accelerate Fe 3+ /Fe 2+ cycle adjacent to the cavity, thus in favor of the decomposition of H 2 O 2 into OH as main reactive oxidizing species. The current catalyst integrates the advantages of homogeneous and heterogeneous advanced oxidation processes and is promising in practical applications.
研究领域:
环境科学
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催化
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化学工程
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Yuanchuan Ren,Jun Wang,Guangfei Qu,Nanqi Ren,Ping Lu,Xiuping Chen,Zuoliang Wang,Yuyi Yang,Yan Hu
Three-dimensional electrochemical reactor (3DER) is an efficient technology for the treatment of printing and dyeing wastewater. The particle electrode between anode and cathode is the core unit of 3DER, which determines the treatment efficiency of wastewater. However, the deactivation of the particle electrode caused by the coverage of the catalytic sites seriously hindered the continuous operation of 3DER. In this work, γ-Fe 2 O 3 @CNTs particle electrode was prepared by immersion calcination , and its performance was evaluated by degradation of Rhodamine B (RhB) wastewater in 3DER. The study showed that in γ-Fe 2 O 3 @CNTs/Mn@FNE-3DER, the removal rate of RhB reached the best of 99.16% within 7 min under the conditions of γ-Fe 2 O 3 @CNTs dosage of 1.00 g·L -1 , initial RhB concentration of 100 mg·L -1 , pH 7.0, and current density of 20 mA·cm −2 . The superior catalytic activity of the system is mainly due to the charge transfer channel in γ-Fe 2 O 3 @CNTs structure, which improves the mass transfer efficiency of electrons. According to LC-MS analysis, the degradation process of RhB can be divided into five stages: deethylation, chromophore cracking, debenzylation and deamination, ring opening and mineralization. Hydroxyl radicals play an important role in this process. After the reaction, most RhB is converted into CO 2 and H 2 O. In addition, the study also showed that the Fe 3+ /Fe 2+ circulating system formed between the anode and cathode was the important reason for the high degradation efficiency of RhB. After five cycles of experiments, the degradation efficiency of 92.55% was still maintained, indicating that the particle electrode has significant stability and reusability in the catalytic process. To sum up, the excellent performance of γ-Fe 2 O 3 @CNTs particle electrode in three-dimensional electrochemical system provides a promising idea for the actual treatment of printing and dyeing wastewater.
研究领域:
环境工程
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电化学
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水处理
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DOI
高影响因子
危险品化学品经营许可证（带存储）