石墨相氮化碳基材料的缺陷调控策略及其光催化性能研究进展

鹿宇; 刘成宝; 郑磊之; 陈丰; 邱永斌; 孟宪荣; 陈志刚

石墨相氮化碳基材料的缺陷调控策略及其光催化性能研究进展

鹿宇^{1, 2},
刘成宝^{1, 2, 3, ,},
郑磊之^{1, 2, 3},
陈丰^{1, 2, 3},
邱永斌⁴,
孟宪荣⁵,
陈志刚^{1, 2, 3}

1.
苏州科技大学　江苏省环境功能材料重点实验室, 江苏苏州 215009
2.
苏州科技大学　材料科学与工程学院, 江苏苏州 215009
3.
江苏水处理技术与材料协同创新中心, 苏州科技大学苏州 215009
4.
江苏省陶瓷研究所有限公司, 江苏宜兴 214221
5.
苏州市环境科学研究所, 江苏苏州 215007

基金项目: 江苏省自然科学基金(BK20180103, BK20180971)；苏州市科技发展计划项目(民生科技—关键技术应用研究)(SS202036)

详细信息

通讯作者:
刘成宝，博士，副教授，硕士生导师，研究方向为二维基催化材料、量子点材料和环境功能材料等的结构设计、合成及其环境和能源性能评价E-mail: Lcb@mail.usts.edu.cn

中图分类号: TB34; TB332
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- HTML全文浏览量: 18
- 被引次数: 0
出版历程
- 收稿日期: 2024-01-05
- 修回日期: 2024-02-29
- 录用日期: 2024-03-09
- 网络出版日期: 2024-04-12

Progress in defect modulation of g-C₃N₄ based materials and its photocatalytic property

LU Yu^{1, 2},
LIU Chengbao^{1, 2, 3
, ,},
ZHENG Leizhi^{1, 2, 3},
CHEN Feng^{1, 2, 3},
QIU Yongbin⁴,
MENG Xianrong⁵,
CHEN Zhigang^{1, 2, 3}

1.
Jiangsu Key Laboratory for Environment Functional Materials, Suzhou University of Science and Technology, Suzhou 215009, China
2.
School of Materials Science and Engineering, Suzhou University of Science and Technology , Suzhou 215009, China
3.
Jiangsu Collaborative Innovation Center of Technology and Material for Water Treatment, Suzhou University of Science and Technology, Suzhou 215009, China
4.
Jiangsu Province Ceramics Research Institute Co., Ltd., Yixing 214221, China
5.
Suzhou Institute of Environmental Science, Suzhou 215007, China

Funds: This work was financially supported by Natural Science Foundation of Jiangsu Province (BK20180103, BK20180971), Suzhou Science and Technology Development Plan Project (Livelihood Science and Technology - Application Research of Key Technology) (SS202036)

摘要

摘要: 半导体光催化材料已成为有效应对环境污染和能源危机关键技术的核心要素。其中，石墨相氮化碳(g-C₃N₄)作为一种新兴的高效催化材料展现出了巨大的应用潜力。然而，未改性的g-C₃N₄存在诸如可见光响应范围有限、活性位点偏少以及光生载流子复合速率高等缺点，严重制约了其实际应用。为了解决上述问题，研究人员采取了多种策略，如设计和开发异质结构、实施缺陷工程和进行形貌调控等。其中，缺陷调控因能有效地调制光催化材料的电子能带结构、延缓载流子的复合和增加表面活性位点等原因备受关注。本文阐述了缺陷修饰的类型、缺陷调控策略，最后对g-C₃N₄基材料的开发和光催化应用进行了总结并给出了展望。
- 缺陷调控 /
- 光催化 /
- 石墨相氮化碳 /
- 调控策略 /
- 半导体 /
- 环境污染
Abstract: Semiconductor photocatalytic materials have become a key factor of photocatalytic technologies to solve environmental pollution and energy crisis. Among them, graphitic phase carbon nitride (g-C₃N₄) has shown great potential for application as an emerging highly efficient catalytic material. However, the unmodified g-C₃N₄ has disadvantages such as limited visible light response range, less reactive sites and high photogenerated carrier complexation rate, which severely limit its practical applications. Thus, researchers have adopted various strategies, such as designing and developing heterogeneous structures, defect engineering and morphological modulation to solve the problems mentioned above. Among them, defect modulation has attracted much attention because it can effectively modulate the electronic band structure of photocatalytic materials, delay carrier recombination and increase the surface reactive sites. This paper describes the types of defect modulations, defect modulation strategies, and finally summarizes the development and application of g-C₃N₄ based photocatalytic materials and gives an outlook.
- defect modulation /
- photocatalysis /
- graphitic carbon nitride /
- modulation strategy /
- semiconductor /
- environmental pollution

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图 1 g-C₃N₄常见缺陷类型的示意图

Figure 1. Schematic diagram of common defect types in g-C₃N₄

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图 2 g-C₃N₄空位缺陷的结构示意图

Figure 2. Structural schematic diagram of vacancy defects in g-C₃N₄

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图 3 (a) CN和CNQ 680的带状结构示意图; (b)转换后的Kubelka-Munk与光能图; (c), (d) CNQs和CN的典型TEM图像^[19]

Figure 3. (a) Schematic band structure of CN and CNQ 680; (b) Converted Kubelka-Munk vs. light energy maps; (c), (d) The typical TEM images of CNQs and CN^[19]

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图 4 (a) K(x)–CN中K离子的可能掺杂位点; (b)所制备的g-C₃N₄和K(x)–CN的带隙结构; (c) g-C₃N₄的SEM图像; (d) K(0.05)–CN的SEM图像^[30]

Figure 4. (a) Possible doping site for K ions in K(x)–CN; (b) Band gap structures of as-prepared g-C₃N₄ and K(x)–CN; (c) SEM images of g-C₃N₄; (d) SEM images of K(0.05)–CN^[30]

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图 5 CN(a)、CN-K2(b)和CN-Na2(c)的晶体结构; (d), (e)分别是(b)和(c)中掺杂层的俯视图(所选距离以pm为单位标记)^[31]

Figure 5. Crystal structures of CN(a)、CN-K2(b) and CN-Na2(c); (d), (e)are top views of the doped layers in(b)and(c)respectively(the selected distances are marked in pm units)^[31]

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图 6 (a)比较g-C₃N₄纳米片、g-C₃N₄纳米片和Fe掺杂g-C₃N₄纳米片在阳光照射下对水溶液中RhB降解的光催化活性; (b)在阳光照射下，Fe掺杂g-C₃N₄纳米片在水溶液中降解RhB的高光催化活性示意图^[33]

Figure 6. (a)Comparison of the photocatalytic activities of bulk g-C₃N₄, and pure and Fe-doped g-C₃N₄ nanosheets for the degradation of RhB in aqueous solution under sunlight irradiation; (b)Schematic diagram of the high photocatalytic activity of Fe-doped g-C₃N₄ nanosheets for the degradation of RhB in aqueous solution under sunlight irradiation^[33]

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图 7 (a) PSN-40的SEM图像; (b)已制备的gCN、SN-650和PSN-40的PL和(c) EIS^[38].

Figure 7. (a) SEM images of PSN-40; PL (b) and EIS (c) of as-prepared gCN, SN-650, and PSN-40^[38].

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图 8 (a)不同温度下合成的缺氮氮化碳的红外光谱^[72]; (b)CN和SCN不同煅烧温度下的EPR光谱^[73]

Figure 8. (a)FTIR spectra of nitrogen-deficient carbon nitride synthesized at different temperatures^[72]; (b)CN and SCN at different calcination temperatures EPR spectra^[73]

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表 1 氮化碳改性的的各种参数和应用

Table 1. Various parameters and applications of carbon nitride modification

Control strategy	Type of defect	Add Substances	E_g/eV	BET/(m² g⁻¹)	Application	Refer
Pre-polymerization adjustment	C_v(carbon vacancy)	Ar	2.79	160	HER	[62]
	C_v(carbon vacancy)	CO₂	2.84	147	No oxidization	[63]
	N_V(nitrogen vacancy)	HNO₃	2.78	421.59	HER, Pollutant removal	[64]
	N_V, —C≡N(nitrogen and Cyanide vacancies	Nabh₄	2.71	53.7	HER	[65]
	N_V(nitrogen vacancy)	Nabh₄	2.66	56.05	No removal	[66]
Polymerization time adjustment	N_V(nitrogen vacancy)	H₂	2.0	－	HER	[67]
	N_V(nitrogen vacancy)	N₂	2.78	67.5	No removal	[68]
	N_V(nitrogen vacancy)	N₂	2.07	65.6	Overall water splitting	[69]
	C_v(carbon vacancy)	Acetone	2.33	153.78	HER	[70]
	C_v(carbon vacancy)	－	2.92	75.24	Nitrogen fixation	[71]
Notes: E_g—Band gap; BET—Specific surface area; HER—Hydrogen evolution reaction

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石墨相氮化碳基材料的缺陷调控策略及其光催化性能研究进展

通讯作者:
刘成宝，博士，副教授，硕士生导师，研究方向为二维基催化材料、量子点材料和环境功能材料等的结构设计、合成及其环境和能源性能评价E-mail: Lcb@mail.usts.edu.cn

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Progress in defect modulation of g-C₃N₄ based materials and its photocatalytic property

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石墨相氮化碳基材料的缺陷调控策略及其光催化性能研究进展

通讯作者: 刘成宝，博士，副教授，硕士生导师，研究方向为二维基催化材料、量子点材料和环境功能材料等的结构设计、合成及其环境和能源性能评价E-mail: Lcb@mail.usts.edu.cn

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Progress in defect modulation of g-C3N4 based materials and its photocatalytic property

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通讯作者:
刘成宝，博士，副教授，硕士生导师，研究方向为二维基催化材料、量子点材料和环境功能材料等的结构设计、合成及其环境和能源性能评价E-mail: Lcb@mail.usts.edu.cn

Progress in defect modulation of g-C₃N₄ based materials and its photocatalytic property