g-C3N4基非金属异质结光催化降解水中有机污染物的研究进展

doi:10.11949/0438-1157.20250293

化工学报 ›› 2025, Vol. 76 ›› Issue (9): 4752-4769.DOI: 10.11949/0438-1157.20250293

g-C₃N₄基非金属异质结光催化降解水中有机污染物的研究进展

赵维¹^,³(), 邢文乐¹^,²(), 韩朝旭¹, 袁兴中²^,³, 蒋龙波²^,³

^1.湖南工商大学资源环境学院，湖南长沙 410205
^2.湘江实验室，湖南长沙 410205
^3.湖南大学环境科学与工程学院，湖南长沙 410082

收稿日期:2025-03-24 修回日期:2025-04-22 出版日期:2025-09-25 发布日期:2025-10-23
通讯作者: 邢文乐
作者简介:赵维（2000—），女，硕士研究生，2239949507@qq.com
基金资助:
湘江实验室重大项目(24XJ01003);湖南省自然科学基金项目(2023JJ30136);湖南省自然科学基金项目(2023JJ40234);湖南省生态环境厅环保科研项目(HB KYXM-2023011);湖南省教育厅科研项目(23B0039);湖南省教育厅科研项目(24B0568)

Progress of g-C₃N₄-based metal-free heterojunction photocatalytic degradation of organic pollutants in water

Wei ZHAO¹^,³(), Wenle XING¹^,²(), Zhaoxu HAN¹, Xingzhong YUAN²^,³, Longbo JIANG²^,³

^1.School of Resource and Environment, Hunan University of Technology and Business, Changsha 410205, Hunan, China
^2.Xiangjiang Laboratory, Changsha 410205, Hunan, China
^3.College of Environmental Science and Engineering, Hunan University, Changsha 410082, Hunan, China

Received:2025-03-24 Revised:2025-04-22 Online:2025-09-25 Published:2025-10-23
Contact: Wenle XING

摘要/Abstract

摘要：

石墨相氮化碳（g-C₃N₄）作为新型非金属光催化剂，凭借其可见光响应和环境兼容性，在有机污染物降解领域备受关注。然而，其本征光生载流子复合率高、光谱吸收范围窄（<460 nm）及表面活性位点不足等缺陷，导致光量子效率低下。通过能带工程优化与界面电荷定向传输，构建异质结体系，可显著提升载流子分离效率并拓宽光响应边界。相较于金属基异质结，g-C₃N₄基非金属体系在避免重金属溶出风险的同时，展现出更优的化学稳定性。然而，关于不同类别非金属材料与g-C₃N₄构成的非金属异质结材料在光催化降解水中有机污染物方面的研究，目前尚缺乏系统的综述。本文综述了不同非金属材料，如碳材料、黑磷、氮化硼、共价有机框架（COF）、苝二酰亚胺（PDI）、氮化碳等分别与氮化碳构建非金属型复合异质结材料的结构特征、构建策略、催化降解效率、机理及其性质，对典型的g-C₃N₄基非金属异质结光催化剂的研究成果进行了系统总结。最后，指出了当前g-C₃N₄基非金属异质结复合材料面临的挑战，并对其未来的发展前景进行了展望。

关键词: 光化学, 催化剂, 降解, 复合材料, 氮化碳, 能带工程, 界面电荷转移, 非金属型异质结

Abstract:

Graphitic carbon nitride (g-C₃N₄), as a novel metal-free photocatalyst, has attracted considerable attention in the field of organic pollutant degradation due to its visible light response and environmental compatibility. However, its defects such as high intrinsic photogenerated carrier recombination rate, narrow spectral absorption range (<460 nm) and insufficient surface active sites lead to low photoquantum efficiency. By optimizing the band structure and directing the interfacial charge transfer, constructing heterojunction systems can significantly enhance the carrier separation efficiency and broaden the light response range. Compared with metal-based heterojunctions, g-C₃N₄-based metal-free systems not only avoid the risk of heavy metal leaching but also exhibit superior chemical stability. However, there is currently a lack of systematic reviews on the research of metal-free heterojunction materials composed of different types of metal-free materials and g-C₃N₄ in the photocatalytic degradation of organic pollutants in water. This paper reviews the structural characteristics, construction strategies, catalytic degradation efficiency, mechanisms, and properties of metal-free composite heterojunction materials formed by different metal-free materials with g-C₃N₄, such as carbon materials, black phosphorus, boron nitride, COF, perylene diimide (PDI), and carbon nitride. Finally, the challenges faced by current g-C₃N₄-based metal-free heterojunction composite materials are pointed out, and their future development prospects are discussed.

Key words: photochemistry, catalyst, degradation, composites, carbon nitride, energy band engineering, interfacial charge transfer, metal-free heterojunction

中图分类号:

X 703

赵维, 邢文乐, 韩朝旭, 袁兴中, 蒋龙波. g-C₃N₄基非金属异质结光催化降解水中有机污染物的研究进展[J]. 化工学报, 2025, 76(9): 4752-4769.

Wei ZHAO, Wenle XING, Zhaoxu HAN, Xingzhong YUAN, Longbo JIANG. Progress of g-C₃N₄-based metal-free heterojunction photocatalytic degradation of organic pollutants in water[J]. CIESC Journal, 2025, 76(9): 4752-4769.

图/表 10

图1 各类异质结中光激发载流子的分离机制[5]

Fig.1 Separation mechanisms of photo-excited charge carriers in various types of heterojunctions[5]

图2 不同维度碳材料的结构特征和性能[15]

Fig.2 The structural features and properties of different dimensional carbon materials[15]

图3 (a) 1N-CDs/CN和ca-CDs/CN催化PMS活化和进一步降解PNP的机理[23]；(b) o-GQDs/C3N4异质结构光催化性能增强的机理[24]

Fig.3 (a) Proposed mechanism for 1N-CDs/CN and ca-CDs/CN catalyzed PMS activation and further PNP degradation[23]；(b) The mechanism of enhanced photocatalytic performance of the o-GQDs/C3N4 heterostructures[24]

图4 BP QD(a)、g-C3N4单胞(b)和BP QD/g-C3N4异质结(c)的HOMO和LUMO部分电荷密度[39]

Fig.4 HOMO and LUMO partial charge densities of (a) BP QD, (b) g-C3N4 singlet and (c) BP QD/g-C3N4 heterojunction[39]

图5 (a)H-g-C3N4/BP QDs杂化物在可见光照射下的光催化降解机理图[40]；(b) 6BP/CN的光催化机理[41]

Fig.5 (a) The proposed photocatalytic mechanism of H-g-C3N4/BP QDs hybrids under visible light irradiation[40]; (b) The photocatalytic mechanism of the 6BP/CN[41]

图6 (a)可见光下BN QDs/BPSCN复合材料光催化机理示意图[43]；(b)BN QDs/UPCN异质结构的光催化机理[44]

Fig.6 (a) Schematic illustration of photocatalytic mechanism for BN QDs/BPSCN composite under visible light irradiation[43]; (b) Proposed photocatalytic mechanisms in BN QDs/UPCN heterostructure[44]

图7 h-BN/g-C3N4复合材料中光生电荷的分离和转移示意图（结合催化过程可能的反应机理）：(a) TC降解；(b) RhB降解[48]

Fig.7 Schematic of the separation and transfer of photogenerated charges in the h-BN/g-C3N4 composites combined with the possible reaction mechanism of the photocatalytic procedure: (a) TC degradation; (b) RhB degradation[48]

图8 (a)CNNS/TPA-COF二维/二维异质结光催化剂的制备示意图；(b)CNNS/TPA-COF-2复合材料在可见光照射下可能的光催化机理示意图[58]

Fig.8 (a) Schematic illustration of the preparation of the CNNS/TPA-COF 2D/2D heterojunction photocatalysts; (b) Schematic illustration of the possible photocatalytic mechanism of the CNNS/TPA-COF-2 composite under visible-lightirradiation[58]

图9 氮化碳基多孔同型Ⅱ型异质结示意图[70]

Fig.9 Schematic illustration of g-C3N4 based porous isotype heterojunction[70]

表1 g-C3N4基非金属异质结光催化降解有机污染物的相关参数对比

Table 1 Comparison of relevant parameters for the photocatalytic degradation of organic pollutants by g-C3N4-based metal-free heterojunctions

异质结	合成方法	污染物	初始浓度/（mg/L）	催化剂用量/mg	光照条件	截止波长/nm	PL/TRPL	降解效率/%	降解时间/min	文献
1N-CDs/CN	超声混合法	PNP	10	50	λ≥420 nm	λ≈452	τ=7.43 ns	95.9	35	[23]
o-GQDs/C₃N₄	一步水热法	MO	10	100	λ≥400 nm	λ≈450	PL↓	96.5	120	[24]
DCN-Cg	热聚合法	BPA	10	50	λ：420~780 nm	λ=580	PL↓	99	60	[29]
3-rGO/g-C₃N₄	热聚合法	MO	20	50	λ≤400 nm	λ=500	PL↓	97.5	60	[30]
GO 3%（质量分数）-CN	热聚合法	MB	30	30	λ≥400 nm	λ=445	PL↓	82.31	60	[31]
GA-CN(30%)	水热共组装法	MB	20	5	λ≥420 nm	λ≈740	PL↓	83.0	180	[32]
CNT/CCN-1	水热法	RhB	15	20	λ：200~800 nm	λ≈500	PL↓	100	80	[36]
H-CN/BPQDs	冰辅助超声	TC	10	20	λ：420~800 nm	λ≈446	PL↓	91	30	[40]
6%BP/OPCN	高温热聚合法	MO	20	50	λ：420~720 nm	λ≈430	τ=27.14 ns	100	15	[42]
6BP/CN	液相外延法	HTC	5	5	λ≤400 nm	λ=518	PL↓	99	30	[41]
h-BN/MCN-5	热聚合法	TC	20	20	λ≥420 nm	λ=465	τ=3.99 ns	94.23	40	[49]
1%（质量分数）BN/C₃N₄	球磨法	RhB	5	100	λ>420 nm	λ=450	PL↓	97.2	50	[50]
7.5 BNC	一步热处理法	RR120	10	30	AM1.5G滤光片	λ≈520	PL↓	87.94	90	[51]
COF/g-C₃N₄	液相辅助研磨法	RhB	10	20	λ>400 nm	λ=484	PL↓	86	90	[55]
TpMa/CN-5	自组装法	TC	20	50	λ>420 nm	λ≈650	τ=6.78 ns	82	120	[56]
CNTD-X	溶剂热法	苯酚	20	30	λ≤420 nm	λ≈600	τ=3.41 ns	99.4	12	[57]
CNTC	热缩聚法	RhB	20	25	λ：420~800 nm	λ≈600	PL↓	99.4	40	[58]
g-C₃N₄/PDI	溶液加工法	苯酚	5	25	λ：254~700 nm	λ≈690	τ=0.75 ns	95.3	300	[64]
1%PDI/GCN	一步亚胺化反应	PNP	10	50	λ：400~680 nm	λ≈451	PL↓	98	45	[65]
CNPC3	热聚合法	ATZ	10	30	λ≤420 nm	λ≈500	τ=4.12 ns	94	60	[67]
PDI/CN/CN	简单热解法	TC	10	50	λ≤400 nm	λ≈510	τ=4.64 ns	89.7	60	[68]
PBCN	热聚合法	SSZ	10	200	λ=450 nm	λ≈470	τ=1.84 ns	96	8	[69]
U3M1	共聚合法	RhB	10	50	λ≤420 nm	λ≈460	PL↓	96	60	[70]

表1 g-C3N4基非金属异质结光催化降解有机污染物的相关参数对比

Table 1 Comparison of relevant parameters for the photocatalytic degradation of organic pollutants by g-C3N4-based metal-free heterojunctions

异质结	合成方法	污染物	初始浓度/（mg/L）	催化剂用量/mg	光照条件	截止波长/nm	PL/TRPL	降解效率/%	降解时间/min	文献
1N-CDs/CN	超声混合法	PNP	10	50	λ≥420 nm	λ≈452	τ=7.43 ns	95.9	35	[23]
o-GQDs/C₃N₄	一步水热法	MO	10	100	λ≥400 nm	λ≈450	PL↓	96.5	120	[24]
DCN-Cg	热聚合法	BPA	10	50	λ：420~780 nm	λ=580	PL↓	99	60	[29]
3-rGO/g-C₃N₄	热聚合法	MO	20	50	λ≤400 nm	λ=500	PL↓	97.5	60	[30]
GO 3%（质量分数）-CN	热聚合法	MB	30	30	λ≥400 nm	λ=445	PL↓	82.31	60	[31]
GA-CN(30%)	水热共组装法	MB	20	5	λ≥420 nm	λ≈740	PL↓	83.0	180	[32]
CNT/CCN-1	水热法	RhB	15	20	λ：200~800 nm	λ≈500	PL↓	100	80	[36]
H-CN/BPQDs	冰辅助超声	TC	10	20	λ：420~800 nm	λ≈446	PL↓	91	30	[40]
6%BP/OPCN	高温热聚合法	MO	20	50	λ：420~720 nm	λ≈430	τ=27.14 ns	100	15	[42]
6BP/CN	液相外延法	HTC	5	5	λ≤400 nm	λ=518	PL↓	99	30	[41]
h-BN/MCN-5	热聚合法	TC	20	20	λ≥420 nm	λ=465	τ=3.99 ns	94.23	40	[49]
1%（质量分数）BN/C₃N₄	球磨法	RhB	5	100	λ>420 nm	λ=450	PL↓	97.2	50	[50]
7.5 BNC	一步热处理法	RR120	10	30	AM1.5G滤光片	λ≈520	PL↓	87.94	90	[51]
COF/g-C₃N₄	液相辅助研磨法	RhB	10	20	λ>400 nm	λ=484	PL↓	86	90	[55]
TpMa/CN-5	自组装法	TC	20	50	λ>420 nm	λ≈650	τ=6.78 ns	82	120	[56]
CNTD-X	溶剂热法	苯酚	20	30	λ≤420 nm	λ≈600	τ=3.41 ns	99.4	12	[57]
CNTC	热缩聚法	RhB	20	25	λ：420~800 nm	λ≈600	PL↓	99.4	40	[58]
g-C₃N₄/PDI	溶液加工法	苯酚	5	25	λ：254~700 nm	λ≈690	τ=0.75 ns	95.3	300	[64]
1%PDI/GCN	一步亚胺化反应	PNP	10	50	λ：400~680 nm	λ≈451	PL↓	98	45	[65]
CNPC3	热聚合法	ATZ	10	30	λ≤420 nm	λ≈500	τ=4.12 ns	94	60	[67]
PDI/CN/CN	简单热解法	TC	10	50	λ≤400 nm	λ≈510	τ=4.64 ns	89.7	60	[68]
PBCN	热聚合法	SSZ	10	200	λ=450 nm	λ≈470	τ=1.84 ns	96	8	[69]
U3M1	共聚合法	RhB	10	50	λ≤420 nm	λ≈460	PL↓	96	60	[70]

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g-C₃N₄基非金属异质结光催化降解水中有机污染物的研究进展

Progress of g-C₃N₄-based metal-free heterojunction photocatalytic degradation of organic pollutants in water

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