Research progress on iron-based composite bismuth oxyhalide magnetic materials for enhanced visible light catalytic treatment of refractory organic wastewater

doi:10.16085/j.issn.1000-6613.2024-0501

Abstract

Abstract:

Visible light catalytic oxidation is an efficient, energy-saving and environmentally friendly refractory organic wastewater treatment technology. The key to the efficiency of wastewater purification is the performance of the catalyst. Bismuth oxyhalide (BiOX, X=Br, Cl, I), as a bismuth-based semiconductor material, has the characteristics of suitable band gap, high stability and low toxicity. This is because the [Bi₂O₂]²⁺ plate and the double halogen atom layer are interlaced to form a four-fold perovskite structure. This special layered structure and broadened energy band structure greatly reduce the recombination of photogenerated electron-hole pairs, but the disadvantages of low quantum efficiency, wide band gap, and difficulty in recycling limit its scale application. Iron-based materials have excellent optical properties and play a role of activating oxidant, and are usually magnetic. The combination of the bismuth oxyhalide and iron-based materials can solve the problem of difficult recovery of bismuth oxyhalide and improve the photocatalytic performance. Therefore, this paper reviewed the types, synthesis methods, catalytic performance and reusability of magnetic materials from bismuth oxyhalide to different iron-based composite bismuth oxyhalide magnetic materials, in order to provide reference for improving the recovery efficiency, reusability and photocatalytic performance of photocatalytic materials. It was expected that the removal efficiency of refractory organic pollutants could reach 80%—100% in the practical engineering application of iron-based composite bismuth oxyhalide magnetic catalyst. In the future, the key to the application of iron-based composite bismuth oxyhalide magnetic materials in printing and dyeing wastewater, pharmaceutical wastewater and organic chemical wastewater was to reduce the cost of materials, innovate modification methods, and put them into practical engineering on a large scale, so as to improve their cost performance and practicability.

Key words: photochemistry, catalyst, degradation, photocatalytic efficiency, material modification, refractory organic wastewater

摘要：

可见光催化氧化是一种高效、节能、环境友好的难降解有机废水处理技术，其净化废水效能的关键是催化剂性能。卤氧化铋（BiOX，X=Br、Cl、I）作为铋基半导体材料，具有带隙适宜、稳定性高和毒性低等特征，这是由于[Bi₂O₂]²⁺平板和双卤素原子层交错形成了四重钙钛矿结构。这种特殊的层状和拓宽能带结构，大大减少了光生电子-空穴对的复合，但量子效率低、带隙宽、难以回收循环利用等缺点限制了其规模性应用。铁基材料有着出色的光学性质和活化氧化剂的作用，通常具有磁性。两者复合后可解决卤氧化铋难回收问题，并提升其光催化性能，因此本文梳理了从卤氧化铋到不同的铁基复合卤氧化铋磁性材料的种类、合成方法、催化性能与重复可利用性，以期为提高光催化材料回收效率、可重复利用性和光催化性能提供参考。期望铁基复合卤氧化铋磁性催化剂在实际工程应用中，可以实现难降解有机污染物去除率80%~100%。未来铁基复合卤氧化铋磁性材料在印染废水、制药废水、有机化工废水中应用的关键是降低材料成本、创新改性方法、大规模投入实际工程等，提高其性价比与实用性。

关键词: 光化学, 催化剂, 降解, 光催化效率, 材料改性, 难降解有机废水

CLC Number:

ZHANG Yiru, HAN Dongmei, MA Weifang. Research progress on iron-based composite bismuth oxyhalide magnetic materials for enhanced visible light catalytic treatment of refractory organic wastewater[J]. Chemical Industry and Engineering Progress, 2025, 44(4): 2258-2273.

张绎如, 韩东梅, 马伟芳. 铁基复合卤氧化铋磁性材料强化可见光催化处理难降解有机废水研究进展[J]. 化工进展, 2025, 44(4): 2258-2273.

Figures/Tables 9

高级氧化技术	反应原理	反应条件	降解率/%	反应时间	运行费用
臭氧氧化法	$O 3 + O H → H O 2 + O 2$ $O 3 + H O 2 → · O H + O 2 + O 2$ $O 3 + N H 3 → Q s$ （含NO₃或NO₂的产物）（pH低时，O₃直接氧化为主） $· O H + N H 3 → Q s$ （含NO₃或NO₂的产物）（pH高时，·OH自由基氧化为主）	—	30~90	≤60min	10~1000CNY/m³
湿式氧化法（WAO）	①链引发： $R H + O 2 → R · + H O O ·$ $R H + O 2 → 2 R · + H 2 O 2$ $2 R H + M → 2 R · + 2 · O H$ ②链传递： $R H + H O · → R · + H 2 O$ $R · + O 2 → R O O ·$ $R O O · + R H → R O O H + R ·$ ③链终止： $R · + R · → R — R$ $R O O · + R · → R O O R$ $R O O · + R O O · → R O H + R 1 C O R 2 + O$ （RH为有机物，M为催化剂）	①环境温度：123~320℃ ②压力：0.5~10.0MPa ③催化剂：富氧气体、O₂	75~90	15~20min	10~1000CNY/m³
芬顿氧化法	$F e 2 + + H 2 O 2 → F e 3 + + O H - + H O · + e a q -$ $F e 3 + + H 2 O 2 → F e 2 + + H O 2 · + H +$ 总反应： $2 H 2 O 2 → O H · + H O 2 · + H 2 O$	①合理控制H₂O₂及铁盐投放量 ②一般要求酸性条件	40~90	1~2h	10~1000CNY/m³
超临界水氧化法（SCWO）	有机化合物 $+ O 2 → C O 2 + H 2 O$ $有机化合物的杂原子 → [O] 酸、盐、氧化物$ $酸 + N a O H → 无机盐$	①水的温度374.3℃ ②压力>22.1MPa	>99.99	<1min	100~10000CNY/m³
光催化氧化法	光催化剂 $+ h v → h + + e -$ $e - + O 2 → · O 2 -$ $· O 2 - + H + → H O 2 ·$ $h + + H 2 O → · O H$ $h + + O H - → · O H$ $· O 2 - / · O H / H O 2 ·$ $+$ 有机污染物 $→ C O 2 + H 2 O$ （hv为光子的能量，h⁺和e^-为空穴和电子）	—	50~100	由光催化剂决定	由光催化剂决定

高级氧化技术	反应原理	反应条件	降解率/%	反应时间	运行费用
臭氧氧化法	$O 3 + O H → H O 2 + O 2$ $O 3 + H O 2 → · O H + O 2 + O 2$ $O 3 + N H 3 → Q s$ （含NO₃或NO₂的产物）（pH低时，O₃直接氧化为主） $· O H + N H 3 → Q s$ （含NO₃或NO₂的产物）（pH高时，·OH自由基氧化为主）	—	30~90	≤60min	10~1000CNY/m³
湿式氧化法（WAO）	①链引发： $R H + O 2 → R · + H O O ·$ $R H + O 2 → 2 R · + H 2 O 2$ $2 R H + M → 2 R · + 2 · O H$ ②链传递： $R H + H O · → R · + H 2 O$ $R · + O 2 → R O O ·$ $R O O · + R H → R O O H + R ·$ ③链终止： $R · + R · → R — R$ $R O O · + R · → R O O R$ $R O O · + R O O · → R O H + R 1 C O R 2 + O$ （RH为有机物，M为催化剂）	①环境温度：123~320℃ ②压力：0.5~10.0MPa ③催化剂：富氧气体、O₂	75~90	15~20min	10~1000CNY/m³
芬顿氧化法	$F e 2 + + H 2 O 2 → F e 3 + + O H - + H O · + e a q -$ $F e 3 + + H 2 O 2 → F e 2 + + H O 2 · + H +$ 总反应： $2 H 2 O 2 → O H · + H O 2 · + H 2 O$	①合理控制H₂O₂及铁盐投放量 ②一般要求酸性条件	40~90	1~2h	10~1000CNY/m³
超临界水氧化法（SCWO）	有机化合物 $+ O 2 → C O 2 + H 2 O$ $有机化合物的杂原子 → [O] 酸、盐、氧化物$ $酸 + N a O H → 无机盐$	①水的温度374.3℃ ②压力>22.1MPa	>99.99	<1min	100~10000CNY/m³
光催化氧化法	光催化剂 $+ h v → h + + e -$ $e - + O 2 → · O 2 -$ $· O 2 - + H + → H O 2 ·$ $h + + H 2 O → · O H$ $h + + O H - → · O H$ $· O 2 - / · O H / H O 2 ·$ $+$ 有机污染物 $→ C O 2 + H 2 O$ （hv为光子的能量，h⁺和e^-为空穴和电子）	—	50~100	由光催化剂决定	由光催化剂决定

种类	材料	合成方法	结合后结构	废水种类	目标污染物	剂量 /g·L^-1	污染物浓度/mg·L^-1	反应时间 /min	降解率/%	参考文献
Fe掺杂BiOX （X=Cl、Br、I）、铁基金属有机骨架与BiOX（X=Cl、Br、I）结合	Fe³⁺/BiOCl	溶剂热法	陷阱能级	印染废水	RhB MO	1	5	RhB：20 MO：80	RhB：99 MO：99	[41]
	Fe(Ⅲ)@BOC NS	溶剂热法	—	印染废水	RhB	0.1	约9.6	15	99.27	[34]
	Fe-BiOCl	水热法	陷阱能级	制药废水	左氧氟沙星（LXV）	0.5	15	60	>95	[40]
	Fe-BiOCl@ Fe-MOF	溶剂热法	环形、 Ⅰ型异质结	印染废水制药废水	RhB TC	0.2	RhB：5 TC：10	90	RhB：99 TC：90.4	[43]
	MIL-53(Fe)/ BiOI	水热和简易共沉淀法	Ⅱ型异质结	制药废水	TC	0.2	25	14	86.21	[42]
铁氧化物与 BiOX（X=Cl、 Br、I）结合	BiOCl/Fe₃O₄	共沉淀法	Ⅰ型异质结	制药废水	卡马西平（CBZ）	0.6	80	60	90.3	[66]
	Fe₃O₄/BiOCl	共沉淀法	超顺磁花状	印染废水	RhB	—	40	30	98	[56]
	BiOCl@Fe₃O₄	共沉淀法	—	制药废水	阿替洛尔（ATL）	0.4	2.5	40	100	[67]
	Fe₃O₄/BiOBr	溶剂热法	微球状	印染废水	刚果红（CR）	1.4	20	240	91.18	[68]
	BiOBr/ Fe₃O₄	溶剂热法	p-n型异质结	农业废水	草甘膦（PMG）	4	100	60	97	[69]
	Fe₃O₄/BiOI	共沉淀法	n-p型异质结	印染废水制药废水	MO 磺胺嘧啶钠盐（SD-Na）	1	20	120	MO：81 SD-Na：79	[70]
	Fe₃O₄/BiOI	共沉淀法	中空的三维微球、异质结	有机化工废水印染废水	BPA RhB	1	BPA：20 RhB：—	BPA：90 RhB：180	BPA：100 RhB：95.1	[54]
磁性双金属氧化物和多铁性质的氧化物与 BiOX（X=Cl、 Br、I）结合	LaFeO₃/BiOBr	水热法	Z型异质结	印染废水	RhB	1	5	30	98.2	[71]
	BiOBr/CoFe₂O₄/GO	水热法	Z型异质结	印染废水	RhB	0.2	30	120	100	[72]
	ZnFe₂O₄/BiOI	水热法	Ⅱ型异质结	印染废水	RhB	0.5	10	70	86.54	[60]
	BiOBr/MnFe₂O₄	无表面活性剂水热合成法	Z型异质结	农业废水印染废水	2,4-D RhB	1	2,4-D：20 RhB：20	80	2,4-D：89.3 RhB：96.5	[58]
	BiFeO₃/BiOI	湿浸渍法	Ⅱ型异质结	印染废水有机化工废水	RhB BPA	1	约3.6	RhB：60 BPA：120	RhB：约100 BPA：约71	[73]
FeWO₄、FeVO₄、FeOOH与 BiOX（X=Cl、Br、I）结合	BiOBr/FeWO₄	水热法	Ⅱ型异质结	制药废水	DOX	1	—	60	90.4	[61]
	α-FeOOH/BiOI	沉淀法	Ⅱ型异质结	印染废水	RhB	0.5	20	20	100	[65]
	FeVO₄/BiOCl	湿浸渍法	Z型异质结	印染废水	RhB	0.5	2	360	99.8	[64]

种类	材料	合成方法	结合后结构	废水种类	目标污染物	剂量 /g·L^-1	污染物浓度/mg·L^-1	反应时间 /min	降解率/%	参考文献
Fe掺杂BiOX （X=Cl、Br、I）、铁基金属有机骨架与BiOX（X=Cl、Br、I）结合	Fe³⁺/BiOCl	溶剂热法	陷阱能级	印染废水	RhB MO	1	5	RhB：20 MO：80	RhB：99 MO：99	[41]
	Fe(Ⅲ)@BOC NS	溶剂热法	—	印染废水	RhB	0.1	约9.6	15	99.27	[34]
	Fe-BiOCl	水热法	陷阱能级	制药废水	左氧氟沙星（LXV）	0.5	15	60	>95	[40]
	Fe-BiOCl@ Fe-MOF	溶剂热法	环形、 Ⅰ型异质结	印染废水制药废水	RhB TC	0.2	RhB：5 TC：10	90	RhB：99 TC：90.4	[43]
	MIL-53(Fe)/ BiOI	水热和简易共沉淀法	Ⅱ型异质结	制药废水	TC	0.2	25	14	86.21	[42]
铁氧化物与 BiOX（X=Cl、 Br、I）结合	BiOCl/Fe₃O₄	共沉淀法	Ⅰ型异质结	制药废水	卡马西平（CBZ）	0.6	80	60	90.3	[66]
	Fe₃O₄/BiOCl	共沉淀法	超顺磁花状	印染废水	RhB	—	40	30	98	[56]
	BiOCl@Fe₃O₄	共沉淀法	—	制药废水	阿替洛尔（ATL）	0.4	2.5	40	100	[67]
	Fe₃O₄/BiOBr	溶剂热法	微球状	印染废水	刚果红（CR）	1.4	20	240	91.18	[68]
	BiOBr/ Fe₃O₄	溶剂热法	p-n型异质结	农业废水	草甘膦（PMG）	4	100	60	97	[69]
	Fe₃O₄/BiOI	共沉淀法	n-p型异质结	印染废水制药废水	MO 磺胺嘧啶钠盐（SD-Na）	1	20	120	MO：81 SD-Na：79	[70]
	Fe₃O₄/BiOI	共沉淀法	中空的三维微球、异质结	有机化工废水印染废水	BPA RhB	1	BPA：20 RhB：—	BPA：90 RhB：180	BPA：100 RhB：95.1	[54]
磁性双金属氧化物和多铁性质的氧化物与 BiOX（X=Cl、 Br、I）结合	LaFeO₃/BiOBr	水热法	Z型异质结	印染废水	RhB	1	5	30	98.2	[71]
	BiOBr/CoFe₂O₄/GO	水热法	Z型异质结	印染废水	RhB	0.2	30	120	100	[72]
	ZnFe₂O₄/BiOI	水热法	Ⅱ型异质结	印染废水	RhB	0.5	10	70	86.54	[60]
	BiOBr/MnFe₂O₄	无表面活性剂水热合成法	Z型异质结	农业废水印染废水	2,4-D RhB	1	2,4-D：20 RhB：20	80	2,4-D：89.3 RhB：96.5	[58]
	BiFeO₃/BiOI	湿浸渍法	Ⅱ型异质结	印染废水有机化工废水	RhB BPA	1	约3.6	RhB：60 BPA：120	RhB：约100 BPA：约71	[73]
FeWO₄、FeVO₄、FeOOH与 BiOX（X=Cl、Br、I）结合	BiOBr/FeWO₄	水热法	Ⅱ型异质结	制药废水	DOX	1	—	60	90.4	[61]
	α-FeOOH/BiOI	沉淀法	Ⅱ型异质结	印染废水	RhB	0.5	20	20	100	[65]
	FeVO₄/BiOCl	湿浸渍法	Z型异质结	印染废水	RhB	0.5	2	360	99.8	[64]

材料	结构	合成方法	废水种类	降解对象	剂量 /g·L^-1	污染物浓度 /mg·L^-1	反应时间 /min	降解率/%	参考文献
三元
BiOI/rGO/Fe₃O₄	类花三维分层异质结	共沉淀法	印染废水	RhB	—	20	180	98	[92]
GO/Fe₃O₄/BiOI	牡丹状	—	印染废水印染废水	RhB MB	1	RhB：约4.8 MB：约3.2	RhB：80 MB：120	RhB：99.2 MB：91.4	[93]
Fe₃O₄@BiOI@AgI	微球状	多步合成法	印染废水有机化工废水	RhB BPA	0.5	RhB：5 BPA：20	60	RhB：90 BPA：>70	[94]
Fe₃O₄/BiOBr/BC	异质结	水解法	制药废水	CBZ	1	10	180	95.51	[78]
CoFe₂O₄/BiOBr/GO	Z型异质结	水热法	印染废水	RhB	0.2	30	120	100	[72]
Fe₃O₄/BiOCl/BiOBr	Z型异质结	溶剂热法	有机化工废水	TC	0.4	40	90	85	[95]
BiOBr/BiOI/Fe₃O₄	三维花状、异质结	共沉淀法	有机化工废水	TBBPA	1	40	90	98.5	[91]
Fe₃O₄/BiOBr/CQDs	Z型异质结	光诱导法/水解法	制药废水	CBZ	0.6	10	120	99.52	[79]
Fe₃O₄/BiOBr@HC	微球状	水热法	制药废水	CBZ	0.6	10	40	100	[77]
BiOBr@SiO₂@Fe₃O₄	微球状	多步合成法	有机化工废水	BPA	1	20	50	87	[96]
Fe₃O₄/Bi₂S₃/BiOBr	纳米球/ 纳米棒/ 纳米片状、异质结	一锅溶剂热法	制药废水制药废水	双氯芬酸（DCF）布洛芬（IBU）	0.6 0.2	DCF:10 IBU:10	DCF:40 IBU:30	DCF:93.81 IBU:96.78	[97]
BiOBr/Fe₃O₄/RGO	n型肖特基结	水热法	印染废水	RhB	0.45	20	60	96	[98]
四元
BiOCl/g-C₃N₄/ Cu₂O/Fe₃O₄	p-n-p型异质结	共沉淀法	制药废水	SME	0.2	约25	Xe灯：60 自然光：120	Xe灯：99.5 自然光：92.1	[84]
Fe₃O₄@SiO₂@Co₃O₄@BiOCl	三维花状	水热法、油浴、离子交换法	印染废水	RhB	0.3077	10	50	98.41	[85]
Fe₃O₄/SiO₂/ MnO₂/BiOBr-Bi	三维花状	水热法	印染废水	MB	0.2308	10	150	95.23	[99]

印染废水

制药废水

h⁺、∙O

2 -

印染废水

制药废水

有机化工废水

农业废水

h⁺、∙O

2 -

3~6次

超顺磁性：20次

多元铁基复合卤氧化铋磁性材料

印染废水

制药废水

有机化工废水

h⁺、∙O

2 -

材料

可处理废水种类

反应活性物种

降解率/%

降解时长

材料成本

循环次数

卤氧化铋 BiOX（X=Cl、Br、I）

印染废水

制药废水

h⁺、∙O

2 -

、∙OH

50~90

1~6h

0.8~14.0CNY/g

重复利用性差，几乎无法循环

二元铁基复合卤氧化铋磁性材料

印染废水

制药废水

有机化工废水

农业废水

h⁺、∙O

2 -

、∙OH、¹O₂

70~100

15min~6h

根据复合材料种类决定

3~6次

超顺磁性：20次

多元铁基复合卤氧化铋磁性材料

印染废水

制药废水

有机化工废水

h⁺、∙O

2 -

、¹O₂、 ∙OH、·OOH、O₂

70~100

40min~3h

根据复合材料种类决定

3~5次

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