异相可见光催化耦合过硫酸盐活化技术在水污染控制中的研究进展

doi:10.11949/0438-1157.20221448

摘要/Abstract

摘要：

近年来，如何有效去除水中难降解污染物成为水污染治理中的难点问题。可见光催化耦合过硫酸盐活化技术是一种新型水处理工艺，有望成为难降解污染物高效去除的新策略。该耦合技术中，可见光、催化剂及过硫酸盐三者之间的协同效应被最大限度开发与利用，极大提升了处理工艺的氧化性能。本文回顾了该工艺中常用的金属基、碳基及复合型光催化材料，分析了光催化剂类型、元素组分、表面性质对体系氧化效能及反应机理的影响；讨论了有关催化剂光学特性（光学吸收、电荷动力学和能带结构）的主要表征方法；总结了不同体系中起主要氧化作用的活性物种及其生成机制；最后综述了该工艺在处理染料、酚类、新型污染物以及细菌灭活等不同场景中的应用，并对未来研究所面临的问题提出了展望。

关键词: 可见光催化, 过硫酸盐, 催化剂, 氧化机理, 水污染控制

Abstract:

In recent years, how to effectively remove refractory pollutants from water has become a key issue in water pollution control. Visible light catalysis coupled with persulfate activation technology is a new water treatment process, which is expected to become a new strategy for the efficient removal of refractory pollutants. In the photocatalysis/persulfate oxidation system, the synergistic effect among light radiation, catalyst and persulfate is exploited to the largest extent, which greatly improves the oxidation performance of the treatment process. In this paper, a variety of commonly used metal-based, carbon-based and composite photocatalysts are introduced, and the effects of photocatalyst type, element composition, and surface properties on photocatalytic activity and mechanism are analyzed. The main characterization methods of optical properties are also discussed. Meanwhile, the major reactive species participating in the oxidation process are summarized. Finally, the application of this process for organic contaminants elimination and bacteria inactivation is reviewed. As well, the opportunities and challenges for future research are prospected.

Key words: visible light photocatalysis, persulfate, catalyst, oxidation mechanism, water pollution control

中图分类号:

X 703

徐银, 蔡洁, 陈露, 彭宇, 刘夫珍, 张晖. 异相可见光催化耦合过硫酸盐活化技术在水污染控制中的研究进展[J]. 化工学报, 2023, 74(3): 995-1009.

Yin XU, Jie CAI, Lu CHEN, Yu PENG, Fuzhen LIU, Hui ZHANG. Advances in heterogeneous visible light photocatalysis coupled with persulfate activation for water pollution control[J]. CIESC Journal, 2023, 74(3): 995-1009.

图/表 7

图1 光催化耦合过硫酸盐活化技术的总结

Fig.1 The diagram of the coupling with photocatalysis and activated-persulfate process

表1 光催化材料表征技术

Table 1 Characterizations of photocatalytic material

表征目的	表征内容	表征仪器	文献
光响应范围	紫外-可见漫反射光谱(UV-Vis DRS)	紫外-可见漫反射光谱仪	[45-46]
光生载流子分离状况	光致发光光谱(PL)	荧光光谱仪	[14-16, 45, 47]
	瞬时光电流(I-t)	电化学工作站	[14-15]
光生载流子分离状况/电荷传输能力	电化学阻抗谱(EIS)	电化学工作站	[34]
	循环伏安曲线(CV)	电化学工作站	[49-50]
光生载流子的寿命	时间分辨光致发光光谱(TRPL)	荧光光谱仪	[34, 48]
禁带宽度	Kubelka-Munk方程式	紫外-可见漫反射光谱仪	[52]
	循环伏安曲线(CV)	电化学工作站	[51]
	密度泛函理论(DFT)	Materials Studio、VASP软件	[54-55]
价带电势	价带XPS能谱	X射线光电子能谱	[34]
导带电势	莫特-肖特基(Mott-Schottky)曲线	电化学工作站	[15, 53]

表2 不同VLP-PS体系中主要活性物质

Table 2 The reactive species in VLP-PS systems

VLP-PS体系	主要活性物质	次要活性物质	反应条件	污染物去除效率	文献
ZnFe₂O₄/g-C₃N₄/PMS/Vis	¹O₂, h⁺	$S O 4 · -$ , ^•OH, $O 2 · -$	0.3 g·L^-1 catalyst, 0.1 mmol·L^-1双酚A, 0.5 mmol·L^-1 PMS, pH 3.5~9.0	>99.7% in 60 min	[16]
g-C₃N₄/PDS/Vis	$O 2 ·$ , h⁺	—	0.5 g·L^-1 catalyst, 5.0 mg·L^-1双酚A, 5.0 mmol·L^-1 PDS, pH 3	100% in 90 min	[25]
g-C₃N₄/PMS/Vis	$O 2 · -$	$S O 4 · -$	0.4 g·L^-1 catalyst, 20 mg·L^-1酸性橙Ⅱ, 0.2 g·L^-1 PMS, pH 3.82	96.3% in 30 min	[27]
Co₃O₄/量子点g-C₃N₄/ PMS/Vis	h⁺, $O 2 · -$ , $S O 4 · -$ , ^•OH	—	0.2 g·L^-1 catalyst, 20 mg·L^-1四环素, 50 mg·L^-1 PMS, pH 6	97.1% in 10 min	[28]
CoAl-LDHs/g-C₃N₄/ PMS/Vis	h⁺	$S O 4 · -$ , ^•OH	0.2 g·L^-1 catalyst, 10 μmol·L^-1磺胺嘧啶, 0.5 mmol·L^-1 PMS, pH 6.0	87.1% in 15 min	[32]
Bi₂O₃/CuNiFe LDHs/ PDS/Vis	$S O 4 · -$ , ^•OH	$O 2 · -$ , h⁺	0.4 g·L^-1 catalyst, 10 mg·L^-1 洛美沙星, 0.74 mmol·L^-1 PDS, pH 6.08	84.6% in 40 min	[33]
MoO₃/g-C₃N₄/PDS/Vis	$O 2 · -$ , h⁺	$S O 4 · -$ , ^•OH	0.6 g·L^-1 catalyst, 10 mg·L^-1 氧氟沙星, 5 mmol·L^-1 PDS, natural pH	94.4% in 120 min	[36]
MIL-53(Fe)/PDS/Vis	$O 2 · -$ , $S O 4 · -$ , ^•OH	—	0.2 g·L^-1 catalyst, 300 mg·L^-1四环素, 8.0 mmol·L^-1 PDS, pH 3.45	99.7% in 80 min	[43]
K-Fe/PDS/Vis	$S O 4 · -$ , ^•OH	—	0.4 g·L^-1 catalyst, 0.1 mmol·L^-1 罗丹明B, 7.0 mmol·L^-1 PDS, pH 5.0	97.0% in 180 min	[53]
TiO₂/AB/PDS/Vis	$S O 4 · -$	^•OH	0.5 g·L^-1 catalyst, 30 mg·L^-1四环素, 3.0 mmol·L^-1 PDS, pH 4.1	93.3% in 120 min	[57]
g-C₃N₄/Fe(Ⅲ)/PDS/Vis	$S O 4 · -$ , ^•OH, $O 2 ·$	—	1.875 g·L^-1 g-C₃N₄ with 0.35 g·L^-1 Fe³⁺, 10 mg·L^-1 苯酚, 0.3 g·L^-1 PDS, natural pH	33% in 90 min	[58]
Co₃O₄/CeO₂/PMS/Vis	$O 2 · -$ , $S O 4 · -$ , h⁺, ^•OH	—	0.5 g·L^-1 catalyst, 5.0 mg·L^-1环丙沙星, 0.1 g·L^-1 PMS, pH 3.45	87.8% in 50 min	[59]
Ag/AgCl@ZIF-8/g-C₃N₄/PMS/Vis	$O 2 · -$ , h⁺	$S O 4 · -$ , ^•OH	0.01 g·L^-1 catalyst, 0.01 g·L^-1 洛美沙星, 2.0 mmol·L^-1 PMS, pH 6.5	87.3% in 60 min	[60]
Bi₁₂O₁₇C_l2/MIL-100(Fe)/PDS/Vis	$O 2 · -$	h⁺, $S O 4 · -$ , ^•OH	0.25 g·L^-1 catalyst, 10 mg·L^-1 双酚A, 2.0 mmol·L^-1 PDS, pH 5.2	99.3% in 60 min	[61]
Ilmenite/PDS/Vis	¹O₂	$O 2 · -$ , $S O 4 · -$	1.0 g·L^-1 catalyst, 5 log₁₀ cfu·ml^-1E.coli, 0.5 mmol·L^-1 PDS, pH 5	100% in 20min	[62]
p(HEA-APTM)-BiOI/ PMS/Vis	h⁺, ¹O₂	$O 2 · -$ , $S O 4 · -$ , ^•OH	2.0 g·L^-1 catalyst, 50 mg·L^-1 对羟基苯甲酸甲酯, 1.5 mmol·L^-1 PMS, pH 3.18	100% in 90min	[63]
γ-Fe₂O₃/MnO₂/PMS/Vis	$O 2 · -$ , h⁺, ¹O₂	$S O 4 · -$ , ^•OH	0.15 g·L^-1 catalyst, 50 μmol·L^-1 环丙沙星, 0.3 g·L^-1 PMS, neutral pH	98.3% in 30 min	[64]
Bi₂MoO₆/PDS/Vis	h⁺, $S O 4 · -$	^•OH	0.5 g·L^-1 catalyst, 20 mg·L^-1 四环素, 4.0 g·L^-1 PDS, pH 4.4	83.0% in 60 min	[65]
CuBi₂O₄/PMS/Vis	h⁺, ¹O₂	$S O 4 · -$ , ^•OH	0.5 g·L^-1 catalyst, 5.0 mg·L^-1环丙沙星, 0.125 g·L^-1 PMS, pH 5.0	> 90% in 30 min	[66]
g-C₃N₄/MnFe₂O₄/graphene/PDS/Vis	h⁺, ^•OH, $O 2 · -$	—	1.0 g·L^-1 catalyst, 20 mg·L^-1 甲硝唑, 0.01 mol·L^-1 PDS, natural pH	94.5% in 60 min	[67]
CuBi₂O₄/MnO₂/PMS/Vis	h⁺, $O 2 · -$	$S O 4 · -$ , ^•OH	0.3 g·L^-1 catalyst, 10.0 mg·L^-1 头孢噻呋, 0.4 g·L^-1 PMS, pH 11.0	93.6% in 40 min	[68]

表2 不同VLP-PS体系中主要活性物质

Table 2 The reactive species in VLP-PS systems

VLP-PS体系	主要活性物质	次要活性物质	反应条件	污染物去除效率	文献
ZnFe₂O₄/g-C₃N₄/PMS/Vis	¹O₂, h⁺	$S O 4 · -$ , ^•OH, $O 2 · -$	0.3 g·L^-1 catalyst, 0.1 mmol·L^-1双酚A, 0.5 mmol·L^-1 PMS, pH 3.5~9.0	>99.7% in 60 min	[16]
g-C₃N₄/PDS/Vis	$O 2 ·$ , h⁺	—	0.5 g·L^-1 catalyst, 5.0 mg·L^-1双酚A, 5.0 mmol·L^-1 PDS, pH 3	100% in 90 min	[25]
g-C₃N₄/PMS/Vis	$O 2 · -$	$S O 4 · -$	0.4 g·L^-1 catalyst, 20 mg·L^-1酸性橙Ⅱ, 0.2 g·L^-1 PMS, pH 3.82	96.3% in 30 min	[27]
Co₃O₄/量子点g-C₃N₄/ PMS/Vis	h⁺, $O 2 · -$ , $S O 4 · -$ , ^•OH	—	0.2 g·L^-1 catalyst, 20 mg·L^-1四环素, 50 mg·L^-1 PMS, pH 6	97.1% in 10 min	[28]
CoAl-LDHs/g-C₃N₄/ PMS/Vis	h⁺	$S O 4 · -$ , ^•OH	0.2 g·L^-1 catalyst, 10 μmol·L^-1磺胺嘧啶, 0.5 mmol·L^-1 PMS, pH 6.0	87.1% in 15 min	[32]
Bi₂O₃/CuNiFe LDHs/ PDS/Vis	$S O 4 · -$ , ^•OH	$O 2 · -$ , h⁺	0.4 g·L^-1 catalyst, 10 mg·L^-1 洛美沙星, 0.74 mmol·L^-1 PDS, pH 6.08	84.6% in 40 min	[33]
MoO₃/g-C₃N₄/PDS/Vis	$O 2 · -$ , h⁺	$S O 4 · -$ , ^•OH	0.6 g·L^-1 catalyst, 10 mg·L^-1 氧氟沙星, 5 mmol·L^-1 PDS, natural pH	94.4% in 120 min	[36]
MIL-53(Fe)/PDS/Vis	$O 2 · -$ , $S O 4 · -$ , ^•OH	—	0.2 g·L^-1 catalyst, 300 mg·L^-1四环素, 8.0 mmol·L^-1 PDS, pH 3.45	99.7% in 80 min	[43]
K-Fe/PDS/Vis	$S O 4 · -$ , ^•OH	—	0.4 g·L^-1 catalyst, 0.1 mmol·L^-1 罗丹明B, 7.0 mmol·L^-1 PDS, pH 5.0	97.0% in 180 min	[53]
TiO₂/AB/PDS/Vis	$S O 4 · -$	^•OH	0.5 g·L^-1 catalyst, 30 mg·L^-1四环素, 3.0 mmol·L^-1 PDS, pH 4.1	93.3% in 120 min	[57]
g-C₃N₄/Fe(Ⅲ)/PDS/Vis	$S O 4 · -$ , ^•OH, $O 2 ·$	—	1.875 g·L^-1 g-C₃N₄ with 0.35 g·L^-1 Fe³⁺, 10 mg·L^-1 苯酚, 0.3 g·L^-1 PDS, natural pH	33% in 90 min	[58]
Co₃O₄/CeO₂/PMS/Vis	$O 2 · -$ , $S O 4 · -$ , h⁺, ^•OH	—	0.5 g·L^-1 catalyst, 5.0 mg·L^-1环丙沙星, 0.1 g·L^-1 PMS, pH 3.45	87.8% in 50 min	[59]
Ag/AgCl@ZIF-8/g-C₃N₄/PMS/Vis	$O 2 · -$ , h⁺	$S O 4 · -$ , ^•OH	0.01 g·L^-1 catalyst, 0.01 g·L^-1 洛美沙星, 2.0 mmol·L^-1 PMS, pH 6.5	87.3% in 60 min	[60]
Bi₁₂O₁₇C_l2/MIL-100(Fe)/PDS/Vis	$O 2 · -$	h⁺, $S O 4 · -$ , ^•OH	0.25 g·L^-1 catalyst, 10 mg·L^-1 双酚A, 2.0 mmol·L^-1 PDS, pH 5.2	99.3% in 60 min	[61]
Ilmenite/PDS/Vis	¹O₂	$O 2 · -$ , $S O 4 · -$	1.0 g·L^-1 catalyst, 5 log₁₀ cfu·ml^-1E.coli, 0.5 mmol·L^-1 PDS, pH 5	100% in 20min	[62]
p(HEA-APTM)-BiOI/ PMS/Vis	h⁺, ¹O₂	$O 2 · -$ , $S O 4 · -$ , ^•OH	2.0 g·L^-1 catalyst, 50 mg·L^-1 对羟基苯甲酸甲酯, 1.5 mmol·L^-1 PMS, pH 3.18	100% in 90min	[63]
γ-Fe₂O₃/MnO₂/PMS/Vis	$O 2 · -$ , h⁺, ¹O₂	$S O 4 · -$ , ^•OH	0.15 g·L^-1 catalyst, 50 μmol·L^-1 环丙沙星, 0.3 g·L^-1 PMS, neutral pH	98.3% in 30 min	[64]
Bi₂MoO₆/PDS/Vis	h⁺, $S O 4 · -$	^•OH	0.5 g·L^-1 catalyst, 20 mg·L^-1 四环素, 4.0 g·L^-1 PDS, pH 4.4	83.0% in 60 min	[65]
CuBi₂O₄/PMS/Vis	h⁺, ¹O₂	$S O 4 · -$ , ^•OH	0.5 g·L^-1 catalyst, 5.0 mg·L^-1环丙沙星, 0.125 g·L^-1 PMS, pH 5.0	> 90% in 30 min	[66]
g-C₃N₄/MnFe₂O₄/graphene/PDS/Vis	h⁺, ^•OH, $O 2 · -$	—	1.0 g·L^-1 catalyst, 20 mg·L^-1 甲硝唑, 0.01 mol·L^-1 PDS, natural pH	94.5% in 60 min	[67]
CuBi₂O₄/MnO₂/PMS/Vis	h⁺, $O 2 · -$	$S O 4 · -$ , ^•OH	0.3 g·L^-1 catalyst, 10.0 mg·L^-1 头孢噻呋, 0.4 g·L^-1 PMS, pH 11.0	93.6% in 40 min	[68]

图2 可见光照射下K-Fe活化PDS降解RhB的机理[53]

Fig.2 Proposed mechanism for RhB degradation in the Vis/K-Fe/PDS process [53]

图3 可见光照射下Co3O4/CeO2活化PMS降解环丙沙星的机理[59]

Fig.3 Possible mechanism for ciprofloxacin degradation in Vis/Co3O4/CeO2/PMS process [59]

图4 可见光/AZCN/PMS体系的反应机理[60]

Fig.4 Proposed mechanism of Vis/AZCN/PMS system[60]

图5 可见光/CuBi2O4/MnO2/PMS体系的反应机理[68]

Fig.5 Proposed mechanism of Vis/CuBi2O4/MnO2/PMS system[68]

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