| Citation: |
CAI Yufu, ZHOU Yanjun, LU Junfeng, et al. Removal of methylene blue by Fenton-like system with alkali-activated montmorillonite supported iron catalyst[J]. Acta Materiae Compositae Sinica, 2023, 40(8): 4601-4612. DOI: 10.13801/j.cnki.fhclxb.20221025.001
|
Heterogeneous Fenton-like system has wide oxidation range and fast reaction speed, which can effectively degrade organic pollutants in wastewater. Meanwhile, it can overcome the drawbacks of traditional homogeneous Fenton technology, such as narrow pH range, catalyst recovery difficulty, and avoiding secondary pollution. Therefore, it is the key to develop heterogeneous Fenton-like catalysts with low cost and high efficiency for the treatment of dye wastewater.
A series of alkali-activated montmorillonite (Alk-MMT) with different structure and acidity were prepared by changing the alkali treatment temperature using cheap natural calcium montmorillonite (Ca-MMT) as raw material. The supported iron catalyst (Fe/Alk-MMT) was prepared by impregnation method using Alk-MMT as the carrier, which combined with HO to form Fenton-like system to remove methylene blue (MB). The materials were characterized by XRD, NH-TPD, XPS, SEM, FT-IR, N adsorption - desorption. The effects of reaction conditions such as reaction temperature, initial pH of solution, HO concentration and catalyst dosage in Fenton-like system on the removal efficiency of MB were investigated by single factor experiment. Combined with the characterization and reaction results, the influence of alkali activation on the structure and acidity of montmorillonite was revealed, and the main factors affecting the removal efficiency of MB in Fenton-like system were elucidated.
The structure and acidity of the montmorillonite are changed due to the dissolution of Si in the Si-O tetrahedron of montmorillonite under alkaline conditions, and the degree of which depends on the alkali treatment temperature. With the increase of alkali treatment temperature, the damage degree of layered structure of montmorillonite is gradually aggravated due to dissolving more Si. The specific surface area and acidity increase first and then decrease, and the average pore size shows the opposite trend. The iron species on Fe/Alk-MMT catalysts mainly exist in the form of α-FeO, and the interaction between Fe and Alk-MMT is increased. The change of structure and acidity of montmorillonite significantly affects the removal performance of MB in Fenton-like system. The Fenton-like system composed of Alk-MMT-100 with the largest specific surface area and acidity supported Fe catalyst (Fe/Alk-MMT-100) exhibits better MB removal performance. The loss amount of Fe in the Fe/Alk-MMT-100 catalyst is the lowest due to the strongest interaction between Fe and Alk-MMT-100. The effects of reaction conditions on the removal efficiency of MB in Fenton-like system are as follows: with the increase of reaction temperature, the removal efficiency of MB increases gradually, but the value increases slowly. When the concentration of HO is low, the removal efficiency of MB increases with the increase of HO concentration, but the removal efficiency of MB decreases with the increase of HO concentration from 0.85 mmol/L to 1.95 mmol/L. With the gradual increase of catalyst dosage, the removal efficiency increases, and it tends to be stable when the catalyst dosage reaches 1.25 g/L. The loss amount of iron in the catalyst increases in low pH of solution, which results in the reaction quickly reaching equilibrium. The removal efficiency of MB can reach more than 98.7% when reacting 300 min in the solution pH of 4.0-9.0. The part active site of used catalyst is covered by MB due to the combined action of adsorption and catalytic oxidation during the reaction process, which leads to the decrease of the activity of the catalyst. After thermal regeneration, the activity of the catalyst can be restored. After repeated regeneration and use for 6 times, the activity still does not decrease, which exhibits good stability.
| [1] |
KANG D, YU X, GE M, et al. Novel Al-doped carbon nanotubes with adsorption and coagulation promotion for organic pollutant removal[J]. Journal of Environmental Sciences,2017,54:1-12. DOI: 10.1016/j.jes.2016.04.022
|
| [2] |
DONG R, CHEN D, LI N, et al. Enhancement of organic pollutants bio-decontamination from aqueous solution using newly-designed Pseudomonas putida-GA/MIL-100(Fe) bio-nanocomposites[J]. Environmental Research,2019,173:237-245. DOI: 10.1016/j.envres.2019.03.052
|
| [3] |
XUE F F, TANG B, BIN L Y, et al. Residual micro organic pollutants and their biotoxicity of the effluent from the typical textile wastewater treatment plants at Pearl River Delta[J]. Science of the Total Environment,2019,657:696-703. DOI: 10.1016/j.scitotenv.2018.12.008
|
| [4] |
CHEN M, WANG N, WANG X, et al. Enhanced degradation of tetrabromobisphenol A by magnetic Fe3O4@ZIF-67 composites as a heterogeneous Fenton-like catalyst[J]. Chemical Engineering Journal,2021,413:127539. DOI: 10.1016/j.cej.2020.127539
|
| [5] |
WU Q, SIDDIQUE M S, YU W. Iron-nickel bimetallic metal-organic frameworks as bifunctional Fenton-like catalysts for enhanced adsorption and degradation of organic contaminants under visible light: Kinetics and mechanistic studies[J]. Journal of Hazardous Materials,2021,401:123261. DOI: 10.1016/j.jhazmat.2020.123261
|
| [6] |
LIU G, ZHANG Y, YU H, et al. Acceleration of goethite-catalyzed Fenton-like oxidation of ofloxacin by biochar[J]. Journal of Hazardous Materials,2020,397:122783. DOI: 10.1016/j.jhazmat.2020.122783
|
| [7] |
宿程远, 郑鹏, 廖黎明, 等. Fe3O4 NPs类芬顿预处理对活性污泥法处理阿莫西林废水的影响[J]. 化工学报, 2018, 69(12):5237-5245.
SU Chengyuan, ZHENG Peng, LIAO Liming, et al. Influence of Fe3O4 NPs heterogeneous Fenton-like pre-treatment on activated sludge technology for treatment amoxicillin wastewater[J]. CIESC Journal,2018,69(12):5237-5245(in Chinese).
|
| [8] |
GAO C, CHEN S, QUAN X, et al. Enhanced Fenton-like catalysis by iron-based metal organic frameworks for degradation of organic pollutants[J]. Journal of Catalysis,2017,356:125-132. DOI: 10.1016/j.jcat.2017.09.015
|
| [9] |
郑宇, 于洁, 李平, 等. 膨润土基类芬顿复合材料的制备及其吸附去除废水中污染物的性能[J]. 复合材料学报, 2022, 39(6):2774-2782.
ZHENG Yu, YU Jie, LI Ping, et al. Preparation of bentonite-based Fenton composite material and its adsorption and removal of pollutants in wastewater[J]. Acta Materiae Compositae Sinica,2022,39(6):2774-2782(in Chinese).
|
| [10] |
KOEKKOEK A J J, XIN H, YANG Q, et al. Hierarchically structured Fe/ZSM-5 as catalysts for the oxidation of benzene to phenol[J]. Microporous and Mesoporous Materials,2011,145(1-3):172-181. DOI: 10.1016/j.micromeso.2011.05.013
|
| [11] |
XIANG L, ROYER S, ZHANG H, et al. Properties of iron-based mesoporous silica for the CWPO of phenol: A comparison between impregnation and co-condensation routes[J]. Journal of Hazardous Materials,2009,172(2-3):1175-1184. DOI: 10.1016/j.jhazmat.2009.07.121
|
| [12] |
AZMI N H M, VADIVELU V M, HAMEED B H. Iron-clay as a reusable heterogeneous Fenton-like catalyst for decolorization of Acid Green 25[J]. Desalination and Water Treatment,2013,52(28-30):5583-5593.
|
| [13] |
ZHAO Y H, WANG Y J, HAO Q Q, et al. Effective activation of montmorillonite and its application for Fischer-Tropsch synthesis over ruthenium promoted cobalt[J]. Fuel Processing Technology,2015,136:87-95. DOI: 10.1016/j.fuproc.2014.10.019
|
| [14] |
ZHAO Y H, HAO Q Q, SONG Y H, et al. Cobalt supported on alkne-activated montmorillonite as an efficient catalyst for Fischer-Tropsch synthesis[J]. Energy & Fuels,2013,27(11):6362-6371.
|
| [15] |
HAO Q Q, LIU Z W, ZHANG B, et al. Porous montmorillonite heterostructures directed by a single alkyl ammonium template for controlling the product distribution of fischer-tropsch synthesis over cobalt[J]. Chemistry of Materials,2012,24(6):972-974. DOI: 10.1021/cm203872m
|
| [16] |
HAN X Y, YAO P P, CHENG C, et al. Preparation and in vivo biodistribution of ultra-small superparamagnetic iron oxide nanoparticles with high magnetic targeting response[J]. Journal of Nanoscience and Nanotechnology,2018,18(2):879-886. DOI: 10.1166/jnn.2018.14110
|
| [17] |
YAN Y Z, TANG H L, WU F, et al. Facile synthesis of Fe2O3@graphite nanoparticle composite as the anode for lithium ion batteries with high cyclic stability[J]. Electrochimica Acta,2017,253:104-113. DOI: 10.1016/j.electacta.2017.09.061
|
| [18] |
HUANG X Y, CAI X, XU D H, et al. Hierarchical Fe2O3@CNF fabric decorated with MoS2 nanosheets as a robust anode for flexible lithium-ion batteries exhibiting ultrahigh areal capacity[J]. Journal of Materials Chemistry A,2018,6(35):16890-16899. DOI: 10.1039/C8TA04341H
|
| [19] |
SHI B F, ZHAO C C, JI Y J, et al. Promotion effect of PANI on Fe-PANI/zeolite as an active and recyclable Fenton-like catalyst under near-neutral condition[J]. Applied Surface Science,2020,508:145298. DOI: 10.1016/j.apsusc.2020.145298
|
| [20] |
YUAN M H, DENG W Y, DONG S L, et al. Montmorillonite based porous clay heterostructures modified with Fe as catalysts for selective catalytic reduction of NO with propylene[J]. Chemical Engineering Journal,2018,353:839-848. DOI: 10.1016/j.cej.2018.07.201
|
| [21] |
THOMMES M, KANEKO K, NEIMARK A V, et al. Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report)[J]. Pure and Applied Chemistry,2015,87(9-10):1051-1069. DOI: 10.1515/pac-2014-1117
|
| [22] |
XUE X F, HANNA K, ABDELMOULA M, et al. Adsorption and oxidation of PCP on the surface of magnetite: Kinetic experiments and spectroscopic investigations[J]. Applied Catalysis B: Environmental,2009,89(3-4):432-440. DOI: 10.1016/j.apcatb.2008.12.024
|
| [23] |
PRADISTY N A, SIHOMBING R, HOWE R F, et al. Fe(III) oxide-modified indonesian bentonite for catalytic photodegradation of phenol in water[J]. Makara Journal of Science,2017,21(1):25-33.
|
| [24] |
MARIA A, DE LEON, JORGE C, et al. Catalytic activity of an iron-pillared montmorillonitic clay mineral in heterogeneous photo-Fenton process[J]. Catalysis Today,2008,133-155:600-605.
|
| [25] |
张森晗, 赵永华, 史兴浩, 等. 核桃壳生物炭负载铁催化降解亚甲基蓝性能研究[J]. 化学研究与应用, 2022, 34(4):897-903. DOI: 10.3969/j.issn.1004-1656.2022.04.026
ZHANG Senhan, ZHAO Yonghua, SHI Xinghao, et al. Catalytic degradation of methylene blue by iron supported on walnut shell biochar[J]. Chemical Research and Application,2022,34(4):897-903(in Chinese). DOI: 10.3969/j.issn.1004-1656.2022.04.026
|
| [26] |
DONG X, LIN Y, REN G, et al. Catalytic degradation of methylene blue by Fenton-like oxidation of Ce-doped MOF[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects,2021,608:125578. DOI: 10.1016/j.colsurfa.2020.125578
|
| [27] |
PAN X, CHENG S, SU T, et al. Fenton-like catalyst Fe3O4@polydopamine-MnO2 for enhancing removal of methylene blue in wastewater[J]. Colloids and Surfaces B: Biointerfaces,2019,181:226-233. DOI: 10.1016/j.colsurfb.2019.05.048
|
| [28] |
LU H, ZHANG L, WANG B, et al. Cellulose-supported magnetic Fe3O4-MOF composites for enhanced dye removal application[J]. Cellulose,2019,26(8):4909-4920. DOI: 10.1007/s10570-019-02415-y
|
| [29] |
IMAMURA K, IKEDA E, NAGAYASU T, et al. Adsorption behavior of methylene blue and its congeners on a stainless steel surface[J]. Journal of Colloid & Interface Science,2002,245(1):50-57.
|
| [30] |
WANG W H, ZHANG W, SUN H B, et al. Enhanced photodynamic efficiency of methylene blue with controlled aggregation state in silica-methylene bule-acetate@tannic acid-iron(III) ions complexes[J]. Dyes and Pigments,2019,160:663-670. DOI: 10.1016/j.dyepig.2018.08.068
|
| [1] | NI Yaqian, HE Zhihai, SHI Jinyan, HE Yifeng, LIU Baoju. Influence of coral waste on the strength and volume stability of cement mortar[J]. Acta Materiae Compositae Sinica, 2024, 41(1): 404-413. DOI: 10.13801/j.cnki.fhclxb.20230506.001 |
| [2] | DUAN Jiashun, PENG Liping, YU Huayang, XU Ling. Research progress on the stability and efficiency of the two-dimensional halide perovskite solar cells[J]. Acta Materiae Compositae Sinica, 2022, 39(5): 1890-1906. DOI: 10.13801/j.cnki.fhclxb.20211118.001 |
| [3] | SHI Jingwei, ZHAO Juan, LIU Chuanjun, LI Dongsheng. Stability of composite stiffened panels in plane shear[J]. Acta Materiae Compositae Sinica, 2020, 37(7): 1590-1600. DOI: 10.13801/j.cnki.fhclxb.20191011.001 |
| [4] | XIE Yanxia, BI Songmei, WANG Dongqiang, MA Mingming, WU Fei. Preparation and dispersion stability of Sb2O3/chloroprene latex composite modified with polyvinyl alcohol[J]. Acta Materiae Compositae Sinica, 2018, 35(9): 2535-2541. DOI: 10.13801/j.cnki.fhclxb.20171128.003 |
| [5] | LI Hui, CHU Guohong, SHI Qiang, GENG Bing, ZHANG Shuxiang. Thermal stability of calcium sulfate whisker modified fluororubber composites[J]. Acta Materiae Compositae Sinica, 2011, 28(4): 58-62. |
| [6] | LI Ming, LI Yuan-qing, FU Shao-yun. Cryogenic mechanical properties and thermal stabil ity of polyimidehybrid f ilms f illed with MMT-TiO2 nano-particles[J]. Acta Materiae Compositae Sinica, 2006, 23(1): 69-74. |
| [7] | WAN Zhi-min, DU Xing-wen, XIE Zhi-min. IMPACT RESPONSE AND STABILITY ANALYSIS OF GLASS-EPOXY CYLINDRICAL SHELL[J]. Acta Materiae Compositae Sinica, 2001, 18(4): 82-86. |
| [8] | SUN Xiao-feng, ZHANG Zhi-min. ANALYSIS OF THE NONLINEAR STABILITY OF COMPOSITE MULTIWEB STRUCTURES[J]. Acta Materiae Compositae Sinica, 2001, 18(3): 119-123. |
| [9] | Zhang Zhimin, Tong Xiaolin, Zhou Chenfu. NONLINEAR STABILITY ANALYSIS OF ARBITRARILY LAMINATED STIFFENED PLATES WITHELASTICALLY SUPPORTED EDGES[J]. Acta Materiae Compositae Sinica, 1995, 12(2): 67-76. |
| [10] | Wen Xuanling, Chen Haoran. THE INFLUENCE OF INPLANE BOUNDARY CONSTRAINTS ON NONLINEAR STABILITY OF COMPOSITE LAMINATES UNDER COMPRESSION LOADING[J]. Acta Materiae Compositae Sinica, 1993, 10(2): 33-38. |
| 1. |
程超，张晨宇，裴志磊，陈正国，周飞，周金利，张辉，孙泽玉，余木火. 双环戊二烯单体预聚增粘及其碳纤维增强复合材料性能评价. 复合材料学报. 2024(01): 155-169 .
 本站查看
| |
| 2. |
郝励. 碳纤维对SiC陶瓷基材料的导热性能影响研究. 化学与粘合. 2024(03): 235-239 .
| |
| 3. |
柯锋，王朝恩. 热压制备的碳纤维复合材料不同温度的机械性能测试. 粘接. 2023(10): 112-114 .
|
Supported by: Beijing Renhe Information Technology Co., Ltd. 
DownLoad: