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磁性硅酸盐纳米材料在光催化降解有机污染物中的研究进展

朱浩 杜春艳 曹姣 周璐 余关龙 严蓉 杨玉

朱浩, 杜春艳, 曹姣, 等. 磁性硅酸盐纳米材料在光催化降解有机污染物中的研究进展[J]. 复合材料学报, 2024, 42(0): 1-12.
引用本文: 朱浩, 杜春艳, 曹姣, 等. 磁性硅酸盐纳米材料在光催化降解有机污染物中的研究进展[J]. 复合材料学报, 2024, 42(0): 1-12.
ZHU Hao, DU Chunyan, CAO Jiao, et al. Research Progress of Magnetic Silicate Nanomaterials for Photocatalytic Degradation of Organic Pollutants[J]. Acta Materiae Compositae Sinica.
Citation: ZHU Hao, DU Chunyan, CAO Jiao, et al. Research Progress of Magnetic Silicate Nanomaterials for Photocatalytic Degradation of Organic Pollutants[J]. Acta Materiae Compositae Sinica.

磁性硅酸盐纳米材料在光催化降解有机污染物中的研究进展

基金项目: 湖南省教育厅重点项目(21A0188);湖南省水利水电勘测设计规划研究总院有限公司,湖南省洞庭湖防洪及水资源保障工程技术研究中心项目(HHPDI-KFKT-202306);湖南省自然科学基金项目(2022JJ30616)
详细信息
    通讯作者:

    杜春艳,博士,副教授,硕士生导师,研究方向为水处理新材料 E-mail:cydu@csust.edu.cn

  • 中图分类号: TB34

Research Progress of Magnetic Silicate Nanomaterials for Photocatalytic Degradation of Organic Pollutants

Funds: Scientific Research Foundation of Hunan Provincial Education Department (21A0188); the Open Research Fund of Science and Technology Innovation Platform of Engineering Technology Research Center of Dongting Lake Flood Control and Water Resources Protection of Hunan Province, Hunan Water Resources and Hydropower Survey, Design, Planning and Research Co., Ltd (HHHPDI-KFKT-202306); Natural Science Foundation of Hunan Province (2022JJ30616)
  • 摘要: 光催化是去除水中难降解有机污染物的有效措施,因其高效的矿化能力而显示出巨大的潜力。然而,大多数光催化剂的实际应用受到其粉末形态的制约,使大规模应用成为一个难题。近年来,磁性硅酸盐复合材料在材料科学中因为其稳定和可回收的特性获得了越来越多的关注。本综述回顾了磁性硅酸盐复合材料作为光催化剂的研究现状,探讨了合成、修饰及其降解机制方面的最新进展。最后,对磁性硅酸盐复合材料的研究结果和未来的挑战进行了展望。

     

  • 图  1  2019-2023年磁性硅酸盐水污染研究论文数量(Web of Science,截至2023年12月20日)

    Figure  1.  Number of Papers on Magnetic Silicate for Degradation of Water Pollutants from 2019-2023 based on “Web of Science” (20 th December 2023).

    图  2  磁性硅酸盐光催化剂的制备流程图[13]

    Figure  2.  The preparation of the magnetic silicate composite materials[13]

    图  3  (a) 室温下的FSZ-ZnSe0 and FSZ-ZnSe3光致发光(PL)光谱[39];(b) 室温下的Bi2WO6, Fe3O4@SiO2@/Bi2WO6 and Fe3O4@SiO2@/Bi2WO6/Bi2S3光致发光(PL)光谱[40]

    Figure  3.  (a) Room-temperature PL spectra of FSZ-ZnSe0 and FSZ-ZnSe3 samples[39]; (b) PL spectrum of Bi2WO6, Fe3O4@SiO2@/Bi2WO6 and Fe3O4@SiO2@/Bi2WO6/Bi2S3 nanoarchitecture[40]

    图  4  磁性硅酸盐材料光催化机制示意图

    Figure  4.  Photocatalytic Mechanism of Magnetic Silicate Materials

    图  5  (a) 磁性硅酸盐材料光-芬顿反应中自由基形成机制[42];(b) Ⅱ型异质结构改性磁性硅酸盐光催化机制图[53];(c) Z型异质结改性磁性硅酸盐构光-芬顿机制图[47];(d) 金属掺杂改性磁性硅酸盐光催化机制图[19];(e) 非金属掺杂改性磁性硅酸盐结构光催化机制图 (f) 菲的化学结构[51]

    Figure  5.  (a) Free Radical Formation Mechanism in Photocatalytic Fenton Reaction of Magnetic Silicate Materials[42]; (b) Photocatalysis mechanism of type II heterojunction modified magnetic silicate [53]; (c) Photocatalysis mechanism of Z-type heterojunction modified magnetic silicate[47]; (d) Photocatalysis mechanism of metal-doped modified magnetic silicate[19]; (e) Photocatalysis mechanism of non-metal-doped modified magnetic silicate structure (f) Chemical structure of phenanthrene[51]

    表  1  磁性硅酸盐复合物的制备方法

    Table  1.   Synthesis methods for magnetic silicate composite

    Composite Synthesis technique Magnetism/
    (emu·g−1)
    Average Size/
    nm
    Ref
    Core Shell Functional shell
    Fe3O4@SiO2 @TiO2 Solvothermal method Stöber method Solvothermal method 44 230 [18]
    Fe3O4@SiO2 @TiO2–Ag Carbon reduction Modifed stöber
    Method
    Multi- method 37 375 [19]
    Fe/Si/Zn–Pr6O11 Co-precipitation method Stöber method Co-precipitation method 13.6 65 [11]
    Fe3O4@SiO2@ZnO/ZnS Solvothermal method Stöber method Multi- method 14 700 [17]
    Fe3O4@SiO2-MnO2 Solvothermal method Sodium silicate water glass Co-precipitation method - 100 [20]
    GO-Fe3O4@SiO2@N-TiO2 Solvothermal method Modified stöber method Crosslinking method 46.2 ~350 [21]
    Fe3O4@SiO2@TiO2/rGO Co-precipitation method Stöber method Self-assembly 14.82 500 [22]
    Notes: GO—graphene oxide; rGO—reduced graphene oxide
    下载: 导出CSV

    表  2  Fe3O4/SiO2的主要制备工艺比较

    Table  2.   Comparison of Main Preparation Processes for Fe3O4/SiO2

    Magnetic silicate preparationMethodSourceReaction conditionsolventAdvantagesRef
    Fe3O4 preparationCo-precipitation
    method
    FeCl3·6 H2O
    FeCl2∙4 H2O
    Stir 1-5 h
    (alkaline
    environment)
    DIEasy to operate, with relatively mild reaction conditions[11, 22, 27, 28]
    solvothermal
    method
    FeCl3·6 H2O200°C
    12-16 h
    EGhigh quality under long duration,
    high temperature, and pressure.
    [17, 18, 21]
    SiO2 wrappingSol-gelTEOSStir
    30 min-10 h
    Ethanol/DIMild conditions, controllable
    components, high purity
    [11, 17, 18, 21-23, 27, 28]
    water glassNa2SiO3Stir 3 h(pH=6)DIcontrollable process,
    Low cost
    [20]
    Notes:DI−Deionized water; EG−Ethylene glycol
    下载: 导出CSV

    表  3  原始光催化剂复合磁性硅酸盐前后的带隙能值对比

    Table  3.   Comparison of band gap energy values before and after composite magnetic silicates

    Catalyst Pre-Synthesis
    Energy/eV
    Post-Synthesis
    Energy/eV
    Ref
    Fe3O4@SiO2@TiO2 3.23 2.1 [18]
    Fe3O4@SiO2@ZnO 3.37 2.21 [33]
    Fe3O4@SiO2@CdS 2.42 1.8 [37]
    Fe3O4@SiO2@TiO2 3.25 2.0 [38]
    下载: 导出CSV

    表  4  未改性磁性硅酸盐复合材料降解有机污染物的应用

    Table  4.   Application of pristine magnetic silicate composite materials in the degradation of organic pollutants

    Composite Target
    pollutant
    Reaction condition (light source; Pollutant
    concentration Photocatalyst dosage; pH)
    Degrading
    efficiency/%
    Reuse
    Efficiency%
    Ref
    Fe3O4/SiO2/TiO2 GMC 150 W UV lamp;
    20 ppm, 195 mg/L; 6.9
    63 min, 94.7 67 / 5 [32]
    Fe3O4@SiO2@TiO2 ketamine 1.5 kW xenon arc lamp;
    0.3 μM; 0.1 g/L; 7
    20 min, 100 91 / 6 [34]
    Fe3O4@SiO2@TiO2 MO UV irradiation (15 W, λ = 365 nm); 10 mg/L;0.25 g/L; - 1.5 h, 93.5 89.3 / 5 [41]
    ZnO@SiO2@Fe3O4/PMS DZ 8 W UV-C lamp; 20 mg/L; 0.3 g/L; 9.0 ± 0.2; 2 mM PMS 1 h, 95 39.3 / 5 [42]
    ZnO@SiO2@Fe3O4/PMS MTN 8 W UV-C lamp; 20 mg/L; 0.3 g/L; 5.5 ± 0.5; 2 mM PMS 1 h, 79.3 63.3 / 5 [43]
    BiOBr/ Fe3O4@SiO2 IBU 8 W Philips (E14) lamp 2 mg/L; 1 g/L; 7 1 h, 100 80 / 5 [35]
    Notes: GMC−Gentamicin; MO−Methyl orange; DZ− diazinon; MTN− malathion; IBU− Ibuprofen
    下载: 导出CSV

    表  5  改性磁性硅酸盐复合材料降解有机污染物的应用

    Table  5.   Application of modified magnetic silicate composite materials in the degradation of organic pollutant

    Modification method Composite Targetpollutant Reaction condition(light source;Pollutant concentration Photocatalyst dosage;pH) Degrading efficiency/% Reuseefficiency/% andcycle times Ref
    Forming heterojunctions Fe3O4@SiO2@ Ag2WO4@Ag2S MB LED lamps +Xenon lamp;30 ppm;1 g/L; 7 2.5 h, 99.9 76 / 5 [46]
    Fe3O4@SiO2/
    Bi2WO6/Bi2S3
    RhB 500 W Xe-arc lamp;20 mg/L; 1 g/L; - 2.5 h, 100 ~100 / 5 [40]
    g-C3N4/TiO2/
    Fe3O4@SiO2
    IBU Eight lamps (8 W, Philips);2 mg L−1; 1 g/L; - 1 h, 98 87 / 3 [47]
    Fe3O4@SiO2@
    ZnO/ZnSe
    RhB 250 W mercury lamp;7 mg/L; 0.3 g/L; - 1 h, 97 90 / 4 [39]
    Metal doping Fe3O4@SiO2@
    ZnO-Ag
    phenol 25 W lamp50 mg/L; 0.2 g/L; pH=3 2.5 h, 98.1 90.1 / 4 [19]
    Fe3O4@SiO2/
    TiO2-m
    RhB 250 W mercury lamp;7 mg/L; 1 g/L; - 2 h, 98.1 96.65 / 5 [45]
    Fe3O4@SiO2@
    Sn-TiO2
    phenol 300 W xenon lamp;20 mg/L; 1 g/L; - 1.5 h, 95 ~95 / 3 [48]
    Fe3O4@SiO2@
    Pt/mTiO2-x
    TC 300 W Hg lamp (365 nm);10 mg/L; 4 g/L; - 40 min, 98.2 85.1 / 5 [49]
    Fe3O4@SiO2@
    N-TiO2
    RhB 500 W xenon lamp;10 mg/L; 3.3 g/L; - 50 min, 98 ~98 / 5 [50]
    Non-metal doping Fe3O4@SiO2@
    N-TiO2
    IBU 9 W CFLs;2 mg/L; 1 g/L; 2 5 h, 94 - [27]
    Fe3O4@SiO2@
    N-TiO2
    PQ LEDs;10 mg/L; 0.4 g/L; 6 3 h, 98.7 86.32 / 8 [28]
    GO-FSNT Phenanthrene 300 W Xe lamp;1 mg/L; 0.1 g/L; - 4 h, 94.9 65.7 / 5 [51]
    Notes: MB−Methylene Blue; RhB−Rhodamine b; IBU− Ibuprofen; TC−Tetracycline; PQ−Paraquat
    下载: 导出CSV
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出版历程
  • 收稿日期:  2023-11-24
  • 修回日期:  2024-01-03
  • 录用日期:  2024-01-20
  • 网络出版日期:  2024-02-28

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