石墨相氮化碳的制备及在染料降解膜中的应用进展

doi:10.16085/j.issn.1000-6613.2024-1291

摘要/Abstract

摘要：

水体染料污染是当下严重威胁人类健康和环境安全的重要问题之一。为克服传统水处理技术在降解效率和持久性方面的局限，结合膜和光催化技术的石墨相氮化碳（g-C₃N₄）光催化膜技术已成为当前的研究热点。本文从g-C₃N₄的结构、性质和催化机理出发，强调了其在大比表面积、可定制结构、稳定性以及光催化效率方面的优势。本文进一步对比了g-C₃N₄不同制备方法的优劣，指出传统热聚合法导致的产物结构密集化问题，以及通过结构优化和协同效应来增强其光催化性能的不同策略。接着，本文还系统介绍了g-C₃N₄光催化膜的制备技术及其在染料降解中的应用，涵盖从自支撑膜、负载膜到杂化膜的演进趋势及各类膜的优劣势对比，展示了其在水处理领域的巨大发展潜力。最后，本文指出g-C₃N₄光催化膜在规模化应用、评价标准确立和复合材料选择方面仍面临挑战。

关键词: 石墨相氮化碳, 光催化, 膜技术, 染料降解, 结构性质

Abstract:

Waterborne dye pollution represents a critical threat to human health and environmental safety at present. To surmount the limitations of traditional water treatment technologies concerning degradation efficiency and sustainability, the graphite phase nitrogen carbide(g-C₃N₄) photocatalytic membranes, which integrate membrane and photocatalytic technologies, have emerged as a focal point of recent research. In this review, the merits and demerits of various g-C₃N₄synthesis methods were summarized, noting the dense structure of products resulting from conventional thermal polymerization and exploring diverse strategies to augment photocatalytic performance via structural optimization and synergistic effects. Subsequently, the manuscript systematically delineated the fabrication techniques of g-C₃N₄ photocatalytic membranes and their applications in dye degradation, covering the evolutionary trends from self-supporting and loaded membranes to hybrid membranes and comparing their respective strengths and weaknesses, thereby demonstrating their significant potential for advancement in water treatment fields. Finally, the paper acknowledged ongoing challenges in the scalable application, establishment of evaluation standards and selection of composite materials for g-C₃N₄ photocatalytic membranes.

Key words: graphitic carbon nitride, photocatalysis, membrane technology, dye degradation, structural properties

中图分类号:

O643.36

曾军建, 杜轶君, 何静, 薛立新. 石墨相氮化碳的制备及在染料降解膜中的应用进展[J]. 化工进展, 2025, 44(10): 5899-5910.

ZENG Junjian, DU Yijun, HE Jing, XUE Lixin. Progress in the synthesis of graphitic carbon nitride and its application in dye degradation membranes[J]. Chemical Industry and Engineering Progress, 2025, 44(10): 5899-5910.

图/表 9

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制备方法	方法介绍	优点	缺点	主要应用场景
水热合成^[25]	在封闭系统中使用水作溶剂，加热和高压合成g-C₃N₄	条件温和，易控制	时间较长，对设备要求高	实验室小批量制备
化学气相沉积^[26]	通过分解气态前体高温下在基板上沉积g-C₃N₄	可控性高，纯度高	成本高，设备复杂	高端应用如半导体行业
等离子体溅射反应沉积^[27]	使用等离子体技术将g-C₃N₄的靶材料溅射到基板上	膜质均匀，结构紧凑	能耗高，设备成本高	用于制备薄膜和涂层
热聚合法	将含氮有机物（如尿素或三聚氰胺）在高温下直接转化	操作简便，成本低，效率高	高温反应造成结构密集化	大规模工业生产、光催化剂制备

制备方法	方法介绍	优点	缺点	主要应用场景
水热合成^[25]	在封闭系统中使用水作溶剂，加热和高压合成g-C₃N₄	条件温和，易控制	时间较长，对设备要求高	实验室小批量制备
化学气相沉积^[26]	通过分解气态前体高温下在基板上沉积g-C₃N₄	可控性高，纯度高	成本高，设备复杂	高端应用如半导体行业
等离子体溅射反应沉积^[27]	使用等离子体技术将g-C₃N₄的靶材料溅射到基板上	膜质均匀，结构紧凑	能耗高，设备成本高	用于制备薄膜和涂层
热聚合法	将含氮有机物（如尿素或三聚氰胺）在高温下直接转化	操作简便，成本低，效率高	高温反应造成结构密集化	大规模工业生产、光催化剂制备

结构优化	方法介绍	优化方法	优点	缺点
剥离处理法	使用物理或化学手段将g-C₃N₄从多层结构剥离成单层纳米片	热氧化蚀刻	简单，成本低；可在室温下操作，适用于大规模生产；通过质子化和层间膨胀简化剥离过程	会引入缺陷，产品收率低；需要适当的溶剂和超声设备；对化学品和处理条件要求高
		超声辅助液体剥离
		化学剥离
模板辅助合成法	依赖于模板来控制g-C₃N₄的二维结构，从而构建特定形态的纳米片	硬模板法	精确控制纳米片的形状和尺寸；环保，避免使用有害化学品	需要使用有害化学品；无法精确控制结构
模板辅助合成法	依赖于模板来控制g-C₃N₄的二维结构，从而构建特定形态的纳米片	软模板法	精确控制纳米片的形状和尺寸；环保，避免使用有害化学品	需要使用有害化学品；无法精确控制结构

结构优化	方法介绍	优化方法	优点	缺点
剥离处理法	使用物理或化学手段将g-C₃N₄从多层结构剥离成单层纳米片	热氧化蚀刻	简单，成本低；可在室温下操作，适用于大规模生产；通过质子化和层间膨胀简化剥离过程	会引入缺陷，产品收率低；需要适当的溶剂和超声设备；对化学品和处理条件要求高
		超声辅助液体剥离
		化学剥离
模板辅助合成法	依赖于模板来控制g-C₃N₄的二维结构，从而构建特定形态的纳米片	硬模板法	精确控制纳米片的形状和尺寸；环保，避免使用有害化学品	需要使用有害化学品；无法精确控制结构
模板辅助合成法	依赖于模板来控制g-C₃N₄的二维结构，从而构建特定形态的纳米片	软模板法	精确控制纳米片的形状和尺寸；环保，避免使用有害化学品	需要使用有害化学品；无法精确控制结构

序号	光催化剂	支撑材料	合成方法	染料污染物	降解性能
1	g-C₃N₄	Al₂O₃^[67]	真空过滤法	MB，5mg/L	120min内99%
2	g-C₃N₄	PAN^[68]	真空过滤法	MB，20mg/L	120min内99%
3	g-C₃N₄	PMMA^[69]	真空过滤法	RhB，10mg/L	180min内83%
4	g-C₃N₄	PVDF^[70]	真空过滤法	RhB，10mg/L	250min内84.24%
5	Fe-POMs/g-C₃N₄	PC^[71]	真空过滤法	MB，10mg/L	80min内98.6%
6	GNPs/g-C₃N₄/GO	PC^[72]	真空过滤法	R6G，4.8mg/L	120min内100%
7	g-C₃N₄	碳纤维布^[73]	热凝聚法	RhB，10mg/L	30min内98%
8	g-C₃N₄	Cu^[34]	热凝聚法	MB，3.2mg/L	120min内85%
9	g-C₃N₄/TiO₂	玻璃^[74]	浸涂法	RhB，5mg/L	180min内31.2%
10	g-C₃N₄/rGO	泡沫镍^[75]	浸涂法	MO，5mg/L	180min内97%
11	GCNS	CCP^[76]	化学气相沉积法	MB，10mg/L	180min内60%
12	CNTs/MCU-C₃N₄/GO	PVDF^[77]	层层自组装法	RhB，10mg/L	100min内98.31%