非金属元素掺杂石墨相氮化碳光催化材料的研究进展

doi:10.16085/j.issn.1000-6613.2022-2180

化工进展 ›› 2023, Vol. 42 ›› Issue (10): 5299-5309.DOI: 10.16085/j.issn.1000-6613.2022-2180

非金属元素掺杂石墨相氮化碳光催化材料的研究进展

宋亚丽¹(), 李紫燕¹, 杨彩荣¹, 黄龙², 张宏忠¹()

^1.郑州轻工业大学材料与化学工程学院，环境污染治理与生态修复河南省协同创新中心，河南郑州 450001
^2.郑州大学生态与环境学院，河南郑州 450001

收稿日期:2022-11-23 修回日期:2023-06-04 出版日期:2023-10-15 发布日期:2023-11-11
通讯作者: 张宏忠
作者简介:宋亚丽（1988—），女，博士，讲师，主要研究方向为光催化技术在水体修复中的应用。E-mail：songyl@zzuli.edu.cn。
基金资助:
国家自然科学基金(22006139);河南省创新型科技团队项目(CXTD2015023)

Research progress of non-metallic element doped graphitic carbon nitride photocatalytic materials

SONG Yali¹(), LI Ziyan¹, YANG Cairong¹, HUANG Long², ZHANG Hongzhong¹()

^1.Henan Collaborative Innovation Center for Environmental Pollution Control and Ecological Restoration, College of Materials and Chemical Engineering, Zhengzhou University of Light Industry, Zhengzhou 450001, Henan, China
^2.College of Ecology and Environment, Zhengzhou University, Zhengzhou 450001, Henan, China

Received:2022-11-23 Revised:2023-06-04 Online:2023-10-15 Published:2023-11-11
Contact: ZHANG Hongzhong

摘要/Abstract

摘要：

石墨相氮化碳（g-C₃N₄）是一种非金属光催化材料，其具有制备成本低、制备过程简单、绿色、无二次污染、带隙能可调控、热稳定性高等特点，使其成为人们在能源与环境领域研究和关注的焦点。然而，g-C₃N₄还存在比表面积小、禁带宽度较大、光生电子和空穴复合过快等缺点，限制了其发展。非金属元素掺杂可以对g-C₃N₄进行改性以有效解决以上问题，使其带隙减小，拓宽光谱响应范围，抑制光生电子-空穴对的复合，提高光吸收能力，来提高其光催化性能。本文对非金属元素掺杂g-C₃N₄的合成方法、应用等方面进行综述，从非金属单元素掺杂（单元素自掺杂和其他单元素掺杂）、非金属多元素共掺杂方面进行了总结。最后指出了在非金属元素掺杂g-C₃N₄方面，仍需要关注g-C₃N₄产量偏低、可见光利用效率不足、回收较难等问题，并强调了非金属元素掺杂g-C₃N₄在治理环境污染和应对能源危机方面的重要作用。

关键词: 石墨相氮化碳, 非金属元素, 掺杂改性, 光催化性能

Abstract:

Graphitic carbon nitride (g-C₃N₄) is a non-metallic photocatalytic material. It has the advantages of low cost, simple preparation process, green, no secondary pollution, adjustable band gap energy and high thermal stability. It has become the research hotspot in the field of energy and environment. However, g-C₃N₄ possesses the disadvantages of small specific surface area, large band gap and fast recombination rate of photogenerated electrons and holes, which limits its application. Non-metallic element doping can effectively solve the above problems by reducing the band gap, broadening the spectral response range, inhibiting the recombination of photogenerated electron-hole pairs and improving the light absorption capacity. In this work, the synthesis methods and application of non-metallic element doped g-C₃N₄ were reviewed. The non-metallic single element doping (single element self-doping and other single element doping) and non-metallic multi-element co-doping were summarized. As for the study on non-metallic element doped g-C₃N₄, it was still necessary to pay attention to the low yield of g-C₃N₄, insufficient utilization efficiency of visible light and reclamation difficulty. The important role of non-metallic element doped g-C₃N₄ in environmental pollution and the energy crisis was also emphasized.

Key words: graphitic carbon nitride (g-C₃N₄), non-metallic doping, doping modification, photocatalytic performance

中图分类号:

TQ314.2

宋亚丽, 李紫燕, 杨彩荣, 黄龙, 张宏忠. 非金属元素掺杂石墨相氮化碳光催化材料的研究进展[J]. 化工进展, 2023, 42(10): 5299-5309.

SONG Yali, LI Ziyan, YANG Cairong, HUANG Long, ZHANG Hongzhong. Research progress of non-metallic element doped graphitic carbon nitride photocatalytic materials[J]. Chemical Industry and Engineering Progress, 2023, 42(10): 5299-5309.

图/表 7

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序号	前体物质	掺杂元素	取代位点	带隙能量(掺杂后/未掺杂)/eV	光催化活性评价指标	去除率或产氢率或产氨率(掺杂后/未掺杂)
1	尿素+咪唑	N	C1	2.26/2.72	罗丹明B去除率	93.5%/47%（提高2倍）^[30]
2	双氰胺+二甲基甲酰胺	C	N3	2.66/2.72	产氢率	8.88μmol·h^-1/1.70μmol·h^-1（提高5.2倍）^[31]
3	氰胺+硫脲	S	N2	—	产氢率	12.16μmol·h^-1/2.03μmol·h^-1（提高6.0倍）^[32]
4	尿素+1-丁基-3-甲基咪唑六氟磷酸盐	P	—	2.31/2.70	四环素去除率	85%/40%（提高2.1倍）^[33]
5	尿素	O	N2	2.78/2.86	磺胺嘧啶去除率	72.64%/38.84%（提高1.8倍）^[34]
6	尿素	O	N1	—	罗丹明B去除率	99%/33%（提高3倍）^[29]
7	硼酸+尿素	B	—	2.44/2.7	亚甲基蓝去除率	86%/11%（提高7.8倍）^[35]
8	尿素+卤化铵	F	N3	2.55/2.78	全氟辛酸去除率	74.3%/57.1%（提高1.3倍）^[36]
9	三聚氯氰+双氰胺+乙腈	Cl	N2	1.78/1.82	罗丹明B去除率	99.6%/16.8%（提高5.9倍）^[37]
10	三聚氰胺+铵盐	Br	层间N	2.75/2.78	土霉素去除率	75%/30%（提高2.5倍）^[38]
11	双氰胺+碘酸钾	I	N2	2.68/2.76	产氨率	200.8mg·L^-1·g^-1/71.9 mg·L^-1·g^-1（提高2.8倍）^[39]

序号	前体物质	掺杂元素	取代位点	带隙能量(掺杂后/未掺杂)/eV	光催化活性评价指标	去除率或产氢率或产氨率(掺杂后/未掺杂)
1	尿素+咪唑	N	C1	2.26/2.72	罗丹明B去除率	93.5%/47%（提高2倍）^[30]
2	双氰胺+二甲基甲酰胺	C	N3	2.66/2.72	产氢率	8.88μmol·h^-1/1.70μmol·h^-1（提高5.2倍）^[31]
3	氰胺+硫脲	S	N2	—	产氢率	12.16μmol·h^-1/2.03μmol·h^-1（提高6.0倍）^[32]
4	尿素+1-丁基-3-甲基咪唑六氟磷酸盐	P	—	2.31/2.70	四环素去除率	85%/40%（提高2.1倍）^[33]
5	尿素	O	N2	2.78/2.86	磺胺嘧啶去除率	72.64%/38.84%（提高1.8倍）^[34]
6	尿素	O	N1	—	罗丹明B去除率	99%/33%（提高3倍）^[29]
7	硼酸+尿素	B	—	2.44/2.7	亚甲基蓝去除率	86%/11%（提高7.8倍）^[35]
8	尿素+卤化铵	F	N3	2.55/2.78	全氟辛酸去除率	74.3%/57.1%（提高1.3倍）^[36]
9	三聚氯氰+双氰胺+乙腈	Cl	N2	1.78/1.82	罗丹明B去除率	99.6%/16.8%（提高5.9倍）^[37]
10	三聚氰胺+铵盐	Br	层间N	2.75/2.78	土霉素去除率	75%/30%（提高2.5倍）^[38]
11	双氰胺+碘酸钾	I	N2	2.68/2.76	产氨率	200.8mg·L^-1·g^-1/71.9 mg·L^-1·g^-1（提高2.8倍）^[39]

序号	前驱体物质	掺杂元素	取代位置	催化活性评价指标	去除率或产氢率			参考文献
序号	前驱体物质	掺杂元素	取代位置	催化活性评价指标	g-C₃N₄	单元素掺杂	多元素共掺杂	参考文献
1	三聚氰胺+六氯三磷腈+硫	P、S	P取代C1位点 S取代N2位点	甲基蓝去除率	58%	69%（P掺杂） 55%（S掺杂）	完全降解	[64]
2	双氰胺+谷胱甘肽	C、O	C取代N1位点 O取代N2位点	产氢率	0.23mmol·h^-1·g^-1	—	18.38mmol·h^-1·g^-1	[65]
3	植酸+三聚氰胺	P、C	—	产氢率	153.9μmol·g^-1·h^-1	—	1493.3μmol·g^-1·h^-1	[67]
4	三聚氰胺+乙醇	C、O	C取代N3位点 O取代N2位点	产氢率	93μmol·g^-1·h^-1	—	395μmol·g^-1·h^-1	[66]
5	双氰胺+尿素+ 四氟硼酸乙基吡啶	B、F	—	产氢率	36μmol·h^-1	—	343.5μmol·h^-1	[69]
6	三聚氰胺+H₂O₂+三硫氰酸	S、O	S取代N2位点 O取代N2位点	罗丹明B去除率	20 %	48%（S掺杂）	75%	[70]
7	三聚氰胺+磷酸铵+氯化铵	P、Cl	P取代C1位点 Cl占据间隙位点	罗丹明B去除率	60%	66.02%（P掺杂） 97.91%（Cl掺杂）	99.62%	[71]
8	硫脲+磷酸氢二胺	S、P	—	罗丹明B去除率	15%	23%（S掺杂）	66%	[72]
9	双氰胺+硝酸+磷酸氢二铵	P、O	—	罗丹明B去除率	13%	37%（O掺杂）	95%	[73]
10	六氯环三磷腈+硫脲	P、S	—	四环素去除率	32.95%	43.48%（P掺杂） 73.50%（S掺杂）	85.85%	[74]
11	三聚氰胺+硫脲+ 磷酸氢二铵	P、S和O	P取代C1位点 O取代N2位点 S占据间隙位点	产氢率	467.33μmol·g^-1·h^-1	574μmol·g^-1·h^-1（S掺杂） 1141μmol·g^-1·h^-1（P掺杂）	2479μmol·g^-1·h^-1	[68]

序号	前驱体物质	掺杂元素	取代位置	催化活性评价指标	去除率或产氢率			参考文献
序号	前驱体物质	掺杂元素	取代位置	催化活性评价指标	g-C₃N₄	单元素掺杂	多元素共掺杂	参考文献
1	三聚氰胺+六氯三磷腈+硫	P、S	P取代C1位点 S取代N2位点	甲基蓝去除率	58%	69%（P掺杂） 55%（S掺杂）	完全降解	[64]
2	双氰胺+谷胱甘肽	C、O	C取代N1位点 O取代N2位点	产氢率	0.23mmol·h^-1·g^-1	—	18.38mmol·h^-1·g^-1	[65]
3	植酸+三聚氰胺	P、C	—	产氢率	153.9μmol·g^-1·h^-1	—	1493.3μmol·g^-1·h^-1	[67]
4	三聚氰胺+乙醇	C、O	C取代N3位点 O取代N2位点	产氢率	93μmol·g^-1·h^-1	—	395μmol·g^-1·h^-1	[66]
5	双氰胺+尿素+ 四氟硼酸乙基吡啶	B、F	—	产氢率	36μmol·h^-1	—	343.5μmol·h^-1	[69]
6	三聚氰胺+H₂O₂+三硫氰酸	S、O	S取代N2位点 O取代N2位点	罗丹明B去除率	20 %	48%（S掺杂）	75%	[70]
7	三聚氰胺+磷酸铵+氯化铵	P、Cl	P取代C1位点 Cl占据间隙位点	罗丹明B去除率	60%	66.02%（P掺杂） 97.91%（Cl掺杂）	99.62%	[71]
8	硫脲+磷酸氢二胺	S、P	—	罗丹明B去除率	15%	23%（S掺杂）	66%	[72]
9	双氰胺+硝酸+磷酸氢二铵	P、O	—	罗丹明B去除率	13%	37%（O掺杂）	95%	[73]
10	六氯环三磷腈+硫脲	P、S	—	四环素去除率	32.95%	43.48%（P掺杂） 73.50%（S掺杂）	85.85%	[74]
11	三聚氰胺+硫脲+ 磷酸氢二铵	P、S和O	P取代C1位点 O取代N2位点 S占据间隙位点	产氢率	467.33μmol·g^-1·h^-1	574μmol·g^-1·h^-1（S掺杂） 1141μmol·g^-1·h^-1（P掺杂）	2479μmol·g^-1·h^-1	[68]

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非金属元素掺杂石墨相氮化碳光催化材料的研究进展

Research progress of non-metallic element doped graphitic carbon nitride photocatalytic materials

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