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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

鹿宇,  刘成宝,  郑磊之,  陈丰,  邱永斌,  孟宪荣,  陈志刚

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文章导航 > 复合材料学报  > 2024 >  41(11): 5603-5619
鹿宇, 刘成宝, 郑磊之, 等. 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[J]. 复合材料学报, 2024, 41(11): 5603-5619. doi: 10.13801/j.cnki.fhclxb.20240320.003
引用本文: 鹿宇, 刘成宝, 郑磊之, 等. 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[J]. 复合材料学报, 2024, 41(11): 5603-5619. doi: 10.13801/j.cnki.fhclxb.20240320.003
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LU Yu, LIU Chengbao, ZHENG Leizhi, et al. Progress in defect modulation of g-C3N4 based materials and its photocatalytic property[J]. Acta Materiae Compositae Sinica, 2024, 41(11): 5603-5619. doi: 10.13801/j.cnki.fhclxb.20240320.003
Citation: LU Yu, LIU Chengbao, ZHENG Leizhi, et al. Progress in defect modulation of g-C3N4 based materials and its photocatalytic property[J]. Acta Materiae Compositae Sinica, 2024, 41(11): 5603-5619. doi: 10.13801/j.cnki.fhclxb.20240320.003
shu

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

doi: 10.13801/j.cnki.fhclxb.20240320.003
  • 1.

    苏州科技大学　江苏省环境功能材料重点实验室，苏州 215009

  • 2.

    苏州科技大学　材料科学与工程学院，苏州 215009

  • 3.

    苏州科技大学 江苏水处理技术与材料协同创新中心，苏州 215009

  • 4.

    江苏省陶瓷研究所有限公司，宜兴 214221

  • 5.

    苏州市环境科学研究所，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

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

  • 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: 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。

     

    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.

     

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  • 图  1  石墨相氮化碳(g-C3N4)常见缺陷类型的示意图

    Figure  1.  Schematic diagram of common defect types in graphitic phase carbon nitride (g-C3N4)

    下载: 全尺寸图片 幻灯片

    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

    下载: 全尺寸图片 幻灯片

    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]

    VB—Valence band; CB—Conduction band

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

    下载: 全尺寸图片 幻灯片

    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 image of g-C3N4; (d) SEM image of K(0.05)-CN[30]

    下载: 全尺寸图片 幻灯片

    图  5  CN (a)、CN-K2 (b)和CN-Na2 (c)的晶体结构；((d), (e))Fig.5(b)和Fig.5(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)) Top views of the doped layers in Fig.5(b) and Fig.5(c), respectively (Selected distances are marked in pm units)[31]

    下载: 全尺寸图片 幻灯片

    图  6  (a) 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罗丹明B (RhB)降解的光催化活性对比；(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, pure and Fe-doped g-C3N4 nanosheets for the degradation of Rhodamine B (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]

    下载: 全尺寸图片 幻灯片

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

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

    下载: 全尺寸图片 幻灯片

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

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

    下载: 全尺寸图片 幻灯片

    表  1  氮化碳改性的各种参数和应用

    Table  1.   Various parameters and applications of carbon nitride modification

    Control strategy Type of defect Add
    substances    		 Eg/eV BET/(m2·g−1) Application Ref.
    Pre-polymerization adjustment Carbon vacancy (Cv) Ar 2.79 160 HER [62]
    Cv CO2 2.84 147 No oxidization [63]
    Nitrogen vacancy (NV) HNO3 2.78 421.59 HER, pollutant removal [64]
    NV, nitrogen and
    cyanide vacancies (—C≡N)    		 NaBH4 2.71 53.7 HER [65]
    NV NaBH4 2.66 56.05 No removal [66]
    Polymerization time adjustment NV H2 2.0 － HER [67]
    NV N2 2.78 67.5 No removal [68]
    NV N2 2.07 65.6 Overall water splitting [69]
    Cv Acetone 2.33 153.78 HER [70]
    Cv － 2.92 75.24 Nitrogen fixation [71]
    Notes: Eg—Band gap; BET—Specific surface area; HER—Hydrogen evolution reaction.
    下载: 导出CSV
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  • 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:  2024-03-21
  • 刊出日期:  2024-11-15

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