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

doi:10.13801/j.cnki.fhclxb.20240204.002

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

doi: 10.13801/j.cnki.fhclxb.20240204.002

朱浩¹,
杜春艳^{1, 2, ,},
曹姣¹,
周璐¹,
余关龙¹,
严蓉¹,
杨玉¹

1.
长沙理工大学　水利与环境工程学院，洞庭湖水环境治理与生态修复湖南省重点实验室，长沙 410114
2.
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，长沙 410007

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(HHHPDI-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；TB332
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- 文章访问数: 191
- HTML全文浏览量: 142
- PDF下载量: 8
- 被引次数: 0
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: 2024-02-06
- 刊出日期: 2024-11-15

Research progress of magnetic silicate nanomaterials for photocatalytic degradation of organic pollutants

ZHU Hao¹,
DU Chunyan^{1, 2
, ,},
CAO Jiao¹,
ZHOU Lu¹,
YU Guanlong¹,
YAN Rong¹,
YANG Yu¹

1.
Key Laboratory of Dongting Lake Aquatic Eco-Environmental Control and Restoration of Hunan Province, School of Hydraulic and Environmental Engineering, Changsha University of Science and Technology, Changsha 410114, China
2.
Engineering Technology Research Center of Hunan Dongting Lake Flood Control and Water Resources Protection of Hunan Province, Hunan Water Resources and Hydropower Survey, Design, Planning and Research CO., LTD.,Changsha 410007, China

Funds: Scientific Research Foundation of Hunan Provincial Education Department (21A0188); 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

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由于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。
- 光催化 /
- 磁性材料 /
- 有机污染物 /
- 硅酸盐 /
- 降解 /
- 废水
Abstract: Photocatalysis is an effective method for removing recalcitrant organic pollutants from water, demonstrating significant potential due to its high mineralization efficiency. However, the practical application of most photocatalysts is hindered by their powder form, posing challenges for large-scale use. Recently, magnetic silicate composite materials have garnered increasing attention in the field of materials science due to their stability and recyclability. In this review, we examine the current state of research on magnetic silicate composite materials as photocatalysts, exploring the latest advancements in synthesis, modification, and degradation mechanisms. Finally, we provide an outlook on the research findings and future challenges associated with magnetic silicate composite materials.
- photocatalysis /
- magnetic materials /
- organic pollutants /
- silicates /
- degradation /
- wastewater

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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” (20th December 2023)

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图 2 磁性硅酸盐光催化剂的制备流程图^[13]

Figure 2. Preparation of the magnetic silicate composite materials^[13]

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图 3 (a) 室温下的FSZ-ZnSe0 and FSZ-ZnSe3的光致发光(PL)光谱^[42]；(b) 室温下的Bi₂WO₆、Fe₃O₄@SiO₂@Bi₂WO₆和Fe₃O₄@SiO₂@Bi₂WO₆/Bi₂S₃的PL光谱^[43]

Figure 3. (a) Room-temperature PL spectra of FSZ-ZnSe0 and FSZ-ZnSe3 samples^[42]; (b) PL spectrum of Bi₂WO₆, Fe₃O₄@SiO₂@Bi₂WO₆ and Fe₃O₄@SiO₂@Bi₂WO₆/Bi₂S₃ nanoarchitecture^[43]

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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

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图 5 (a) 磁性硅酸盐材料光-芬顿反应中自由基形成机制^[40]；(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^[16]；(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^[40]; (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^[16]; (e) Photocatalysis mechanism of non-metal-doped modified magnetic silicate structure; (f) Chemical structure of phenanthrene^[51]

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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.
Composite	Core	Shell	Functional shell
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	[14]
Fe₃O₄@SiO₂@TiO₂	Solvothermal method	Stöber method	Solvothermal method	44	230	[15]
Fe₃O₄@SiO₂@TiO₂-Ag	Carbon reduction	Modifed stöber method	Multi-method	37	375	[16]
Fe₃O₄@SiO₂-MnO₂	Solvothermal method	Sodium silicate water glass	Co-precipitation method	–	100	[17]
GO-Fe₃O₄@SiO₂@N-TiO₂	Solvothermal method	Modified stöber method	Crosslinking method	46.2	~350	[18]
Fe₃O₄@SiO₂@TiO₂/rGO	Co-precipitation method	Stöber method	Self-assembly	14.82	500	[19]
Notes: GO—Graphene oxide; rGO—Reduced graphene oxide.

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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 preparation	Method	Source	Reaction condition	Solvent	Advantage	Ref.
Fe₃O₄ preparation	Co-precipitation method	FeCl₃·6H₂O FeCl₂∙4H₂O	Stir 1-5 h (Alkaline environment)	DI	Easy to operate, with relatively mild reaction conditions	[11, 19, 24-25]
Fe₃O₄ preparation	Solvothermal method	FeCl₃·6H₂O	200°C 12-16 h	EG	High quality under long duration, high temperature, and pressure	[14-15, 18]
SiO₂ wrapping	Sol-gel	TEOS	Stir 30 min-10 h	Ethanol/DI	Mild conditions, controllable components, high purity	[11, 14-15, 18-25]
SiO₂ wrapping	Water glass	Na₂SiO₃	Stir 3 h (pH=6)	DI	Controllable process, low cost	[17]
Notes：DI—Deionized water; EG—Ethylene glycol.

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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	[15]
Fe₃O₄@SiO₂@ZnO	3.37	2.21	[33]
Fe₃O₄@SiO₂@CdS	2.42	1.8	[35]
Fe₃O₄@SiO₂@TiO₂	3.25	2.0	[36]

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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 μmol/L, 0.1 g/L, 7	20 min, 100	91/6	[34]
BiOBr/Fe₃O₄@SiO₂	IBU	8 W Philips (E14) lamp, 2 mg/L, 1 g/L, 7	1 h, 100	80/5	[37]
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	[39]
ZnO@SiO₂@Fe₃O₄/PMS	DZ	8 W UV-C lamp, 20 mg/L, 0.3 g/L, 9.0±0.2, 2 mmol/L PMS	1 h, 95	39.3/5	[40]
ZnO@SiO₂@Fe₃O₄/PMS	MTN	8 W UV-C lamp, 20 mg/L, 0.3 g/L, 5.5±0.5, 2 mmol/L PMS	1 h, 79.3	63.3/5	[41]
Notes: GMC—Gentamicin; MO—Methyl orange; DZ—Diazinon; MTN—Malathion; IBU—Ibuprofen.

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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	Target pollutant	Reaction condition (Light source; Pollutant concentration; Photocatalyst dosage; pH)	Degrading efficiency	Reuse efficiency/ Cycle 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	[43]
	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	[42]
Metal doping	Fe₃O₄@SiO₂@ZnO-Ag	Phenol	25 W lamp; 50 mg/L; 0.2 g/L; pH=3	2.5 h, 98.1%	90.1%/4	[16]
	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/mTiO_2-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%	–	[24]
	Fe₃O₄@SiO₂@N-TiO₂	PQ	LEDs; 10 mg/L; 0.4 g/L; 6	3 h, 98.7%	86.32%/8	[25]
	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.

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