改性g-C3N4光催化降解双酚A的研究进展

doi:10.16085/j.issn.1000-6613.2023-1914

摘要/Abstract

摘要：

光催化技术可源源不断地利用清洁的太阳能来实现对内分泌干扰物双酚A（BPA）的有效降解，从而在众多降解方法中脱颖而出。类石墨相氮化碳（g-C₃N₄）作为经典的半导体材料，具有合成简单、热稳定性和化学稳定性好、经济无污染等优点，广泛应用于光催化降解领域。但是本体g-C₃N₄由于高的光生电子-空穴对复合率、较窄的可见光吸收范围以及较低的氧化电位，使得其降解BPA的性能大大降低。为了提高g-C₃N₄对BPA的降解能力，研究者采用多种改性方法对g-C₃N₄进行改性。本文主要综述了元素掺杂、形貌调控、异质结的构建以及共聚等手段对g-C₃N₄进行改性的进展，从电子结构、能带结构和光学性能等角度出发，详细总结了改性后g-C₃N₄对BPA的降解性能以及降解机理；其次，总结了BPA常见的降解路径及安全性分析；最后针对改性g-C₃N₄降解BPA的有效选择性进行了展望。

关键词: 光催化, 降解, 双酚A, 类石墨相氮化碳, 改性, 机理, 降解路径

Abstract:

Photocatalysis technology can continuously use clean solar energy to achieve effective degradation of the endocrine disruptor, bisphenol A (BPA), which stands out among many degradation methods. Graphite-like carbon nitride (g-C₃N₄), as a classic semiconductor material, has the advantages of simple synthesis, good thermal and chemical stability, economic and pollution-free, and is widely used in the field of photocatalytic degradation. However, due to the high recombination rate of photogenerated electron hole pairs, weak visible light absorption range and low oxidation potential of bulk g-C₃N₄, the performance of BPA degradation by bulk g-C₃N₄ is not high. In order to improve the degradation ability of g-C₃N₄ to BPA, a variety of modification methods are used to modify g-C₃N₄. This paper mainly reviewed the modification of g-C₃N₄ by means of element doping, morphology control, heterojunction construction and copolymerization. From the perspective of electronic structure, band structure and optical properties, the degradation performance and mechanism of modified g-C₃N₄ for BPA were summarized in detail. Secondly, the common degradation pathways and safety analysis of BPA were also summarized. Finally, effective selectivity for the degradation of BPA by modified g-C₃N₄ was prospected.

Key words: photocatalysis, degradation, bisphenol A, g-C₃N₄, modification, mechanism, degradation pathway

中图分类号:

TQ426

马香港, 丁远, 张俊格, 刘应良, 徐慎刚, 曹少魁. 改性g-C₃N₄光催化降解双酚A的研究进展[J]. 化工进展, 2024, 43(11): 6271-6292.

MA Xianggang, DING Yuan, ZHANG Junge, LIU Yingliang, XU Shengang, CAO Shaokui. Progress of photocatalytic degradation of bisphenol A by modified g-C₃N₄[J]. Chemical Industry and Engineering Progress, 2024, 43(11): 6271-6292.

图/表 31

图1 BPA的化学结构

图2 g-C3N4的结构模型[37]

图3 质量分数40% OA-g-C3N4光催化降解BPA的机理[41]

图4 OPCN在可见光照射下对水溶液中BPA的光降解机理[43]（白、红、灰和蓝色球体分别代表H、O、C和N元素）

图5 CE光催化剂[44]

图6 CN和C1.0CN的能带及C1.0CN在可见光照射下降解BPA溶液的机理[45]

图7 CNS活化PMS和光催化降解BPA的建议机理[46]

图8 gCN-P光催化剂[47]

图9 Ag/mpg-C3N4 的光催化降解BPA机理[55]

图10 SA-CoCN光催化机理[56]

图11 MCN的制备及TEM表征[57]

图12 CNQDs/Bi3.64Mo0.36O6.55纳米复合材料增强光催化活性的可能机理[72]

图13 CNNTs形成过程[53]

图14 LiCl-CN形貌及光催化反应机理[74]

图15 未使用酸（a，e）、硝酸（b，f）、盐酸（c，g）、醋酸（d，h）处理的g-C3N4纳米片TEM和SEM图[76]

图16 中空球体和多层壳结构制备[78-79]

图17 MCNS的SEM和TEM图像[71]

图18 CeO2/CNNS的e-/h+转移机理[90]

表1 基于g-C3N4的Ⅱ型异质结光催化剂降解BPA的性能

光催化剂	异质结类型	光源条件	催化剂使用量/mg	BPA浓度/mg·L^-1	性能	参考文献
g-C₃N₄/BiOI	Ⅱ	氙灯300W，λ>400nm	50	20	60min降解100%	[92]
C₃N₄/Bi₄O₅I₂	Ⅱ	氙灯300W，λ>400nm	50	10	60min降解100%	[93]
D35-TiO₂/g-C₃N₄	Ⅱ	氙灯300W，λ>400nm	50	10	15min降解100%	[94]
N-KTiNbO₅/g-C₃N₄	Ⅱ	氙灯300W，λ>420nm	100	2	120min降解100%	[95]
g-C₃N₄/BiOCl _x I_1-_x	Ⅱ	氙灯500W，λ>420nm	30	10	40min降解100%	[96]
g-C₃N₄/BiOBr	Ⅱ	氙灯300W，λ>420nm	10	10	120min降解96.6%	[81]
BiOCl_0.75I_0.25/g-C₃N₄	Ⅱ	氙灯500W，λ>420nm	10	10	60min降解100%	[97]
In₂O₃/g-C₃N₄	Ⅱ	氙灯，λ>420nm	50	50	180min降解91%	[98]

图19 Z型异质结光催化剂在光照射下的电子-空穴分离[83]

图20 C3N4-Zn/BWO异质结对BPA的降解机理以及C3N4-ZN/BWO系统中光生载流子分离和转移[99]

图21 CNB150催化剂的SEM和TEM图像及用于增强有机污染物处理的Z型g-C3N4/BiPO4反应机理[100]

图22 Bi2WO6/g-C3N4/BPQDs双Z型异质结对BPA的降解机理及光生载流子分离和转移[101]

图23 g-C3N4/BiOI/CdS双Z型异质结光催化剂[102]

表2 基于g-C3N4的Z型异质结光催化剂降解BPA的性能

光催化剂	异质结类型	光源条件	催化剂使用量/mg	BPA浓度 /mg·L^-1	性能	参考文献
g-C₃N₄/Bi/γ-Bi₂O₃	全固态Z型	氙灯500W，λ>420nm	20	15	240min降解70.1%	[103]
AgBr/Ag/g-C₃N₄@NGA	全固态Z型	氙灯500W，λ>420nm	70	10	120min降解92%	[104]
CQDs/g-C₃N₄/BiOBr	全固态Z型	LED30W，峰值波450nm，色温6297K	30	15	60min降解92%	[105]
Fe₂O₃-ZnO@C/g-C₃N₄	全固态Z型	氙灯500W	200	10	60min降解92%	[106]
Au/g-C₃N₄/Co₃O₄	直接Z型	氙灯500W，λ>420nm	40	15	150min降解90.3%	[107]
CeO₂/g-C₃N₄	直接Z型	氙灯500W，λ>400nm	40	15	150min降解94.1%	[108]
BiOBr/g-C₃N₄	直接Z型	氙灯300W，λ>420nm	100	5	100min降解100%	[109]
g-C₃N₄/Bi₄O₇	直接Z型	氙灯500W，λ>420nm	80	20	100min降解100%	[110]
α-Fe₂O₃/g-C₃N₄	直接Z型	氙灯500W	20	15	180min降解91.1%	[111]
Ag₃PO₄/g-C₃N₄	直接Z型	─	5	10	180min降解92.8%	[112]
Bi₁₂O₁₅Cl₆@W₁₈O₄₉@g-C₃N₄/PDI	直接Z型	氙灯300W，λ>300nm	18	10	30min降解100%	[113]
g-C₃N₄@CoFe₂O₄/Fe₂O₃	直接Z型	氙灯500W，λ>400nm	10	30	80min降解98.1%	[114]
Ag₃PO₄/g-C₃N₄	直接Z型	氙灯300W，λ>420nm	10	10	80min降解100%	[115]
Uio-66-NH₂/g-C₃N₄	直接Z型	氙灯300W，λ>400nm	10	20	60min降解100%	[116]

图24 g-C3N4/BiO1.2I0.6异质结的示意图[可见光照射下内生电场（IEF）诱导的电荷转移和S型异质结的形成][117]

图25 CN-CeO2的能带结构和光催化机理[118]

图26 2D层状复合材料与其他类型复合材料的比较[119]

图27 UCN-TDA的结构及光催化反应机理[124]

图28 BPA的不同降解路径

图29 BPA和降解产物P1-P19的生物累积因子、致突变性及发育毒性

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改性g-C₃N₄光催化降解双酚A的研究进展

Progress of photocatalytic degradation of bisphenol A by modified g-C₃N₄

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