INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Yifan Wang,Mengyun Zhao,Ting Wang,Mengzhu Li,Xilei Lu,Bingchi Li
Environmental application of cornstalk and production of hydrogen from biomass are two vital research topics. Herein, a low-cost easy preparing strategy was proposed for trying to give a solution. Non-noble metal of Fe ion was used as an oxidizing agent and electron stockpile carrier for degrading cornstalk and providing e − to the cathode. Using proton exchange electrolysis technique, it can realize H 2 production with a Faraday Efficiency of 94.65%. Different influence factors including temperature, electrolytic potential and electrolytic current density were studied. To the degradation products , the preliminary analyses by SEM, FT-IR, GC-MS and 2D HSQC NMR were given. The results demonstrate that Fe 3+ /Fe 2+ -cornstalk electrolytic system could give a new pathway for environmental application of cornstalk and production of hydrogen.
研究领域:
环境科学
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生物能工程
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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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产品关联
DOI
PubMed
高影响因子
Journal of Cleaner Production
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2022
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IF 11.072
Linxuan Xie,Tianshu Zhang,Xinyu Wang,Wenxin Zhu,Zhaoli Liu,Manshun Liu,Jing Wang,Liang Zhang,Ting Du,Chengyuan Yang,Mingqiang Zhu,Jianlong Wang
Semiconductor-based photocatalyst , whose efficiency distinctly hinges on the separation of photoinduced charge transfer within the interface of bulk structure, has incurred some intractable issues due to the existing energy barrier. Regulating the structure of MOF reasonably would feature an accelerated charge separation, and an effective utilization of photogenerated charges. Herein, a new type of MOF with both interior linker and metal valence modulation (m-MIL-101–1.0) is reported to boost photocatalytic activity owing to the formed charge migration pathway. At first, we introduced defective sites via CTAB, which acted as exposed sites for further reduction reaction. Then, NaBH 4 was used to achieve metal valence regulation. Benefiting from the unique structure, the Fe 3+ /Fe 2+ redox center was considered as a driving force to facilitate the charge transfer. It is properly considered that the activity improvement is attributed to the synergistic effect of both internal and external charge transfer channels. As a result, such m-MIL-101–1.0 has a higher activity than that of MIL-101 for photocatalytic degradation of tetracycline in water. We envision this interior configuration would be an ideal paradigm for tuning the activity of MOFs and extending the boundaries of MOF-based photocatalysts.
研究领域:
材料科学
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环境科学
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化学
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产品关联
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
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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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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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xi Chen,Yunfeng Chen,Songrong Li,Cheng Xue,Dongfang Liu,Wenli Huang
Phthalic acid esters (PAEs) pose serious health risks to humans and are difficult to remove by conventional sewage treatment processes. Herein, Fe 2 Mo 3 O 8 /MoO 2 /Mo 2 N composite (FMON) derived from bimetallic organic framework was used to activate peroxymonosulfate (PMS) for dibutyl phthalate (DBP) degradation. FMON exhibited an excellent catalytic effect with DBP removal efficiency of 92.4 % within 60 min. Mo 2 N showed a superior ability in promoting Fe 3+ /Fe 2+ redox cycle. The reduction efficiencies of Fe 3+ by Mo 2 N/MoO 2 composite and MoO 2 were 67 %–94 % and 11 %–23 %, respectively, in the homogeneous comparative experiment. Moreover, the ratio of Fe 2+ /Fe 3+ in FMON increased significantly after the catalytic reaction. Fe element doping also enhanced the reuse stability and reduced the metal ion leaching of the catalyst. The degradation of DBP was mediated by a variety of reactive species, of which SO 4 − , OH and O 2 − were dominant. Fe element, Mo element and O vacancies were confirmed to exert significant contributions as active sites in the catalytic process. Three degradation pathways of DBP were obtained by DFT calculation and HPLC-MS analysis. And the toxicity of DBP degradation products was significantly reduced based on the assessment result of Toxicity Estimation Software Tool (T.E.S.T.). This study explored a novel Fe/Mo bimetallic catalyst with friendly Fe 3+ /Fe 2+ cycling for environmental catalysis and provided new ideas for the treatment of PAEs wastewater.
研究领域:
环境催化
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废水处理
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材料科学
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产品关联
DOI
高影响因子
Materials Today Communications
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2023
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IF 3.8
Siyuan Zhang,Xinjian Cheng
Developing water-soluble fluorescent probes has important scientific and practical significance. In this work, coumarin derivatives bearing -OH were obtained through the classical Knoevenagel reaction firstly. Secondly, -C C- on allyl bromide was introduced into coumarin by Williamson ether formation method. Thirdly, hydrazine hydrate was added to the coumarin derivatives, a polymerizable small molecular coumarin fluorophore containing probe was obtained successfully. And, the -COOH on di-thioester underwent an esterification reaction with –OH groups on β-cyclodextrin(β-CD) to prepare oligomer based reversible addition-fragmentation chain transfer(RAFT) reagents. Finally, three copolymer probes β-CD-PMAA-Coumarin, β-CD-PMAm-Coumarin, and β-CD-PHEMA-Coumarin were prepared via RAFT polymerization , in which C C-coumarin was used as the functional monomer and methacrylamide(MAm)/methacrylic acid (MAA)/hydroxyethyl methacrylate (HEMA) as the main monomers. The MALDI-TOF mass tests showed that the macromolecular level probes were successfully prepared. These polymer probes have molecular weights up to 5.4 kDa and have narrow molecular weight distributions (PDI≤1.31). With the assistance of water-soluble long-chained PMAm/PMAA/PHEMA and hydrophilic β-CD, the coumarin containing macromolecular fluorescent probes could be dissolved in water readily. These water soluble polymer fluorescent probes could recognize Fe 3+ /Fe 2+ and Cu 2+ ions with high sensitivity. The detection limit of Fe 3+ could be as low as 0.34 μM. This study successfully developed a promising technique for producing highly selective, fully water-soluble fluorescent macromolecular probes.
研究领域:
化学
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材料科学
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分析化学
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产品关联
DOI
高影响因子
JOURNAL OF 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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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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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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产品关联
DOI
高影响因子
CHEMOSPHERE
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2024
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IF 8.1
Yunzhan Ying,Shikun Liang,Fayang Zhang,Xiangwei Xu,Chenbo Qian,Long Jiang,Jing Zhou,Yulong Wan,Lie Wang,Yuyuan Yao
The harmful impact of organic pollutants on aquatic ecosystems underscores the pressing need for effective remediation. While activating peroxymonosulfate (PMS) with Fe catalyst offers a promising approach for eliminating these pollutants, its widespread use is hindered by the sluggish regeneration of Fe 2+ from Fe 3+ . Here, this study demonstrates for the first time that combining an Fe catalyst with Mo 2 C (Fe-Mo 2 C) enhances the Fe³⁺/Fe 2 ⁺ cycle, thereby improving PMS activation. The Fe-Mo 2 C/PMS system achieved near-complete degradation of carbamazepine (CBZ) within only 8 minutes, with an impressive observed rate constant ( k obs ) of up to 0.624 min -1 , about 15 times greater than that of Fe-C catalyst. It also exhibits the capability to degrade a broad range of common antibiotics, phenols, and dye-like organic compounds. Through electron paramagnetic resonance (EPR) analysis and quenching experiments, it was verified that hydroxyl radicals (·OH), sulfate radicals (SO 4 ·- ), singlet oxygen ( 1 O 2 ), and superoxide radicals (·O 2 - ) species during the reaction, with the former three serving as the primary active species. These findings offer a hopeful avenue for the systematic development and enhancement of catalysts specifically designed to efficiently remediate organic pollutants in wastewater.
研究领域:
环境科学
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化学工程
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催化
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水处理
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）