JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2015
·Vol. 91
·期 4
·985-993
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IF 2.349
Jiang Lu,Xiaodan Wei,Yu Chang,Shuanghong Tian,Ya Xiong
BACKGROUND An ozonation catalyst needs to be recycled easily and to exhibit high activity in view of its practical application in wastewater treatment. In this study, magnetic mesoporous MgFe 2 O 4 was successfully prepared and used as a new ozonation catalyst for degradation of Acid Orange II (AOII). The role of Mg in MgFe 2 O 4 was revealed to explain the high activity by catalytic experiments and XPS analysis. RESULTS The degradation efficiency of AOII in the MgFe 2 O 4 /O 3 process exceeds 90% over a wide pH range of 4.6–9.6, slightly affected by the solution pH. The catalytic activity of MgFe 2 O 4 is much higher than that of MgO, Fe 2 O 3 and also their mixture (MgO+Fe 2 O 3 ) with identical molar ratio of Mg 2+ to Fe 3+ , indicating the first role of Mg, i.e. coupling with Fe to present a synergistically catalytic effect. Furthermore, MgFe 2 O 4 possesses a reaction rate constant at least 2.3 times that of NiFe 2 O 4 , MnFe 2 O 4 , and CuFe 2 O 4 . It illustrates the second role of Mg, i.e. causing the high electron density on lattice oxygen in MgFe 2 O 4 indicated by XPS and thus favoring activation of the electrophilic ozone. CONCLUSIONS This study demonstrated the easy recycling and high activity of MgFe 2 O 4 in catalytic ozonation, and revealed the role of Mg in MgFe 2 O 4 . © 2015 Society of Chemical Industry
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
CARBON
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2021
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IF 9.594
Chao Zhang,Huifeng Dong,Binling Chen,Tianxu Jin,Jun Nie,Guiping Ma
The development of bifunctional activity and long durability of ORR/OER catalyst is vital for realizing the practical application of Zn–air batteries (ZAB). Herein, 3D-structured bifunctional catalysts , CoFe nanoalloy decorated carbon nanotubes (CNT) anchoring with 2D MXene (Fe/Co-CNT@MXene-T), were prepared and fabricated as the cathode for both aqueous and flexible ZAB. Taking advantages of active sites of CoFe nanoparticles , robust sheath and fast charge transfer provided by CNT and MXene, our optimal catalyst Fe/Co-CNT@MXene-8 exhibited remarkable electroactivities of ORR and OER comparable with the benchmark Platinum carbon (Pt/C) and Ruthenium dioxide (RuO 2 ), respectively. The as-assembled aqueous ZAB with Fe/Co-CNT@MXene-8 as cathode exhibited a high specific capacity of 759 mA h g −1 at a current density of 10 mA cm −2 , and a stable voltage platform in the quick discharge–charge test under a 375h long-lasting operation, superior to those assembled with benchmark commercial catalyst and other reported catalysts. Furthermore, the as-assembled flexible ZAB with Fe/Co-CNT@MXene-8 as cathode also presented excellent durability cycling and showed promising perspectives as future power sources for wearable application. Such high performance was also verified by X-ray absorption near-edge structure (XANES) and supported by density functional theory (DFT) calculation. This work provides a novel view to design highly effective and long-lasting rechargeable ZABs.
研究领域:
材料科学
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电化学
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能源技术
✓ 已验证
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
Weirui Chen,Muxin Lin,Jiaxin Zhou,Xukai Li,Xipeng Wei,Gaozu Liao,Jing Wang,Laisheng Li
Lewis acid site was vital center for activating O 3 during catalytic ozonation process. Herein, we proposed a strategy to enhance the Lewis acid strength of Fe-MCM-48 (FeM) by fluorination. Fluorinated Fe-MCM-48 (FFeM) exhibited the better catalytic ozonation efficiency towards Ketoprofen (KET), a kind of nonsteroidal anti-inflammatory drug. 87.4 % TOC removal was obtained by F 2.5 Fe 0.8 M/O 3 process, but only 27.5 % and 52.7 % were found by sole ozonation and Fe 0.8 M/O 3 processes, respectively. Comparative characterizations, experiments and DFT calculations showed that fluorinated FFeM was regular sphere with three dimensional duct channel and large S BET . Doping of F reduced particle size, implanted electron withdrawing Si-F group and formed the electron poor center around Fe atom, which enhanced Lewis acid strength of FFeM. Protonated hydroxyl groups on Lewis acid sites were the main active sites for O 3 activation. Greater amount of O 3 were absorbed on the surface of FFeM and the greater O 3 utilization rate, •OH and •O 2 – generation rates were obtained by FFeM/O 3 process. Common anions such as Cl − , SO 4 2− and NO 3 – and Humic acids (HA) had little effect on KET removal but inhibited TOC removal in FFeM/O 3 process. •OH, •O 2 – and Fe(IV) = O oxidation were accounted for KET degradation. 16 kinds of intermediates generated from KET degradation and 4 pathways were deduced.
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
Journal of Water Process Engineering
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2024
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IF 6.3
Zhenggang Huang,Chuanming Zhang,Chunyang Shen,Lili Jin,Yaxiong Zeng,Baohong Guan
Ammonia nitrogen (NH 4 + -N) is one of the regular indexes and the most important contaminants in drinking water. However, it is still a great challenge to remove low concentration NH 4 + -N from drinking water in a safe way. Here we used NaX zeolite and alkali-modified NaX zeolite (NaX-A) as adsorbents and catalysts for ozonation to remove NH 4 + -N in water without adding any chemicals. The zeolites present significant adsorption of NH 4 + -N with Freundlich adsorption affinity of 2.10–3.27 mg 1-n ·L -n ·g −1 by ion-exchange on the bridged Si-O-Al groups. The NaX-A catalytic ozonation achieves 26.7 % of NH 4 + -N removal and up to 75.0 % of gaseous products selectivity in 20 min. The NH 4 + -N oxidation rate constant is raised by 10.7 times over O 3 /NaX-A compared with single ozonation. The alkali modification stimulates the formation of acid sites in NaX-A, and thus improve the adsorption of NH 4 + -N and the decomposition of O 3 into hydroxyl radicals (·OH) for the conversion of NH 4 + -N to gaseous products. This study provides new insights into catalytic ozonation by alkali-modified zeolites to remove NH 4 + -N in water via coupling adsorption with catalytic ozonation.
研究领域:
环境科学
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化学工程
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水处理技术
✓ 已验证
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
Tao Xu,Meihui Jiang,Xuhui Mao,Falak Sher,Tianlin Ren,Kun Xin,Irshad Hussain,Helin Hua,Xu Wang
This study investigated the important role of hydroxyl groups for the preparation of γ-Al 2 O 3 sphere supported metal catalysts. γ-Al 2 O 3 spheres were calcinated at varied temperatures for the analysis of surface hydroxyl group, and they were subsequently loaded with iron to evaluate the metal dispersion and the performance for catalytic ozonation. The results showed that the critical site for metal anchoring was hydroxyl group, thus a higher hydroxyl group content favored the metal dispersion on γ-Al 2 O 3 spheres; meanwhile, the iron-loaded catalysts prepared by the γ-Al 2 O 3 support calcinated at 300 °C achieved the highest catalytic efficiency for p -nitrophenol degradation (74.6 %). The favorable performance of the catalyst was attributed to the excellent dispersion of iron oxide particles, and the abundant oxygen vacancy sites that facilitated the formation of ozone-activating sites, Fe-centered hydroxyl groups ([Fe-OH]). This study provides an important theoretical guidance for the design and application of ozone catalysts.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2019
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IF 5.107
Pengwei Yan,Jimin Shen,Lei Yuan,Jing Kang,Binyuan Wang,Shengxin Zhao,Zhonglin Chen
Si-doped α-Fe 2 O 3 by controlling the atom ratio of Si/Fe was synthesized for catalytic ozonation of nitrobenzene in aqueous solution. Basing on the results of batch oxidation experiments, the catalysts in Si/Fe ratios of 0.1, 0.5, 1.0, and 2.0 showed various activities for ozone decomposition into hydroxyl radical ( OH), which obviously enhanced the removal efficiency of nitrobenzene in aqueous solution compared with sole ozonation. The best Si/Fe ratio was 0.5 in present study. The dose of the catalyst, solution pH and reaction temperature can significantly affect the removal efficiency of nitrobenzene. Moreover, the catalyst was composed of Si–Fe binary oxides and α-Fe 2 O 3 . With the increase of Si/Fe ratio, the surface relative content of Si-Fe binary oxides increases and the relative content of α-Fe 2 O 3 decreases, which promotes the ozone adsorption-desorption on the surface of the catalyst. The generation of hydroxyl radical in catalytic ozonation was dependent on the synergy of ozone adsorption-desorption by Si–Fe binary oxides and ozone decomposition by α-Fe 2 O 3 on the surface of the catalyst.
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
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
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2023
·Vol. 106
·期 7
·4089-4102
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IF 3.9
Peng Zhao,Yuanhui Gao,Guogang Xu,Enliang Zhang,Lulu Liu,Shaowei Jin
In this experiment, a novel catalytic ceramic membrane (CCM) with spherical Cu 1.4 Mn 1.6 O 4 material loading was prepared through hydrothermal in situ growth method. The synergistic effects of membrane separation and catalytic ozonation on membrane antipollution and degradation of micro-pollutants were systematically investigated. The results indicated that the degradation efficiency of bisphenol A by CCMs reached 85.7% with a stable normalized flux of 0.90 under the operating conditions of [O 3 ] = 4 g/h, transmembrane pressure = 0.2 bar, and pH = 6. In addition, the results showed that the composite bimetallic oxides have good stability by measuring the leaching concentration of metal ions during the catalytic process. This study provides a promising strategy for in situ growth of catalytically active composite bimetallic oxides on the surfaces of ceramic membrane and for mitigation of membrane fouling complex water 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
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Jian Guan,Yuqi Liu,Qiuyi Zhu,Guojun Ma,Jiayu Zhang,Zheyong Fan,Wei Chen,Jiawei Yang,Ning Han,Yunfa Chen
At present, near-ground ozone still acts as an air pollutant, posing threats to human’s health. In this study, Fe-based catalysts with different coordination environments and valance states were synthesized and the coordination environments were verified using EXAFS and XRD Rietveld fitting, while in-situ Raman and in-situ DRIFTs were employed to investigate the oxygen intermediates of ozone catalytic reaction. The following activities order for ozone catalytic reaction was obtained: [FeO 6 ] 3+ ≫ [FeO 4 ] 3+ > [FeO 6 ] 2+ ≈ [FeO 4 ] 2+ proven by DFT calculations, and α-Fe 2 O 3 with [FeO 6 ] 3+ coordination structure has a high efficiency of about 80 % after 2 h at a WHSV of 720000 mL g -1 h −1 and ozone concentration of 1000 ppm. The superior catalytic activity could be attributed to the high crystal splitting energy in the octahedral coordination structure, which could offer electrons easily for the catalytic reaction. This study provides valuable insights for the development of Fe-based ozone catalysts as well as for other transition metal oxides.
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 MATERIALS SCIENCE
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2024
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IF 3.5
Ma Shuwen,Zhu Binji,Gan Ruihui,Wang Yue,Zhou Bangguo,Shi Jingli,Song Yan,Shao Xiaodong,Ma Chang
The development of highly active non-precious metal bifunctional oxygen catalysts is of great significance in improving the efficiency of zinc-air batteries (ZABs). In this work, Co 3 O 4 is modified by a simple sulfur-doping strategy, which achieves a sulfur-doped Co 3 O 4 (S-Co 3 O 4 ) with significantly-enhanced oxygen catalytic activity. The doping of sulfur promotes the exposure of cobalt active sites and brings abundant oxygen vacancies, which provide additional active sites and enhance the conductivity of Co 3 O 4 . Consequently, S-Co 3 O 4 exhibits a low overpotential of 318 mV in the oxygen evolution reaction (OER) and an improved half-wave potential (0.788 V) for oxygen reduction reaction (ORR). In addition, the sulfur doping increases the ORR kinetic current density of pristine Co 3 O 4 by a factor of 49. The assembled ZABs based on S-Co 3 O 4 cathodes show a higher peak power density (98.90 mW cm −2 ) than the commercial Pt/C + RuO 2 -based ZABs. This work reveals that the intrinsic oxygen catalytic activity of Co 3 O 4 can be significantly strengthened by sulfur doping, which can modify its structural characteristics and introduce structural defects. Graphical abstract
研究领域:
材料科学
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能源科学
✓ 已验证
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
Dongyao Yue,Zhe Wang,Jing Chang,Shaopo Wang,Jingjie Yu,Hongying Meng,Rui Zhang
In the O 3 self-decomposition process, the poor HO 2 − formation efficiency limits O 3 decomposition and •OH production. Although the addition of Fenton’s reagent facilitates this process, H 2 O 2 consumption and Fe(III) sedimentation must be addressed. In this study, carbon-coated Fe 3 O 4 (Fe 3 O 4 @C) samples were prepared using the metal–organic frameworks (MOFs) modification method for the catalytic ozonation of aromatics, which effectively solved the above challenges. The fabricated 4-Fe 3 O 4 @C catalyst not only exhibited a yolk-shell structure, but also increased •OH production by 9-fold, resulting in optimal target removal, mineralization, and O 3 decomposition efficiency. Further investigation confirmed that the activity of 4-Fe 3 O 4 @C was owing to the combined action of Fe(II) on the catalyst surface and the H 2 O 2 produced from aromatic degradation. Furthermore, the outer carbon layer with reducing properties regenerated Fe(II) in a timely manner, ensuring catalyst durability. Finally, a clear pathway for enhancing O 3 decomposition and •OH generation is proposed.
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
Water
·
2023
·Vol. 15
·期 21
·3801
·
IF 3.4
Yaoji Chen,Ruifu Chen,Xinglan Chang,Jingying Yan,Yajie Gu,Shuang Xi,Pengfei Sun,Xiaoping Dong
In order to realize the high value-added reuse of coal fly ash, a reusable Fe-modified fly ash catalyst was synthesized for ozone catalysis degradation of chemical oxygen demand (COD) in wastewater. Through enhancement of the pretreatment procedure and FeOxmodification, the resulting fly ash with Fe modification demonstrated increased specific surface area and porosity. The presence of Fe loading significantly enhances the reactivity of surface oxidizing reactive species, particularly oxygen vacancy, leading to improved adsorption and activation properties towards ozone molecules. Sodium acetate is chosen as a probe for contaminants due to its status as a small organic substance that remains resistant to further direct oxidation by ozone. This makes it suitable for evaluating the catalyst’s effectiveness in degrading chemical oxygen demand (COD). The quantitative detection of free radicals revealed the generation of •O2−was nearly 10 times that of •OH and dominated the reaction. This study showcases the potential of fly ash, an industrial byproduct, to be utilized as a cost-effective and easily prepared catalyst with consistent physical and chemical characteristics.Keywords:coal fly ash catalyst;iron oxide;ozone catalysis;radical oxidation;COD degradation
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Chen-Yan Hu,Ye-Ye Zhu,Bin Xu,Tian-Yang Zhang,Yi-Li Lin,Cun Xiong,Qiang-Bing Wang,Dan-Dan Huang,Ling Xu
This study explored the degradation of an iodine X-ray contrast media , iohexol, under heterogeneous ozone-catalyzed oxidation by adding Fe 3 O 4 and 1-hydroxybenzotriazole (HBT). Results show that increasing the dosages of Fe 3 O 4 catalyst and ozone as well as solution pH were beneficial to the degradation of iohexol. The presence of low background humic acid (HA) concentration (≤10 mg/L) promoted iohexol degradation, but high HA concentration (≥20 mg/L) inhibited it. Adding HBT exhibited a similar effect on iohexol degradation as HA. The degradation rate constant of iohexol was calculated as 0.07108 min −1 in the Fe 3 O 4 /O 3 /HBT process ([HBT] = 5 μM) at pH 7.0, which was approximately 1.5 times higher than that in the Fe 3 O 4 /O 3 process (0.04533 min −1 ), and 4 times higher than that in the O 3 process (0.01742 min −1 ). Fe 3 O 4 /O 3 /HBT process was pH-dependent with high degradation efficiency of iohexol at pH 5 or 7. Singlet oxygen ( 1 O 2 ), hydroxyl radical ( OH ∙ ), and superoxide radical ( O 2 - ∙ ) have been identified in the Fe 3 O 4 /O 3 /HBT process, and the conversion of Fe 2+ to Fe 3+ was more obvious on the surface of Fe 3 O 4 compared to that in the Fe 3 O 4 /O 3 process. Transformation intermediates were identified, and the degradation pathways of iohexol were proposed. Overall, Fe 3 O 4 /O 3 could enhance iohexol degradation compared with ozone-only system, and adding trace HBT in Fe 3 O 4 /O 3 system can further enhance heterogeneous ozone-catalyzed process for rapid organic matter degradation.
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
危险品化学品经营许可证（带存储）