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化学进展 2022, Vol. 34 Issue (4): 898-908 DOI: 10.7536/PC210401 前一篇   后一篇

• 综述 •

二维纳米材料g-C3N4在电化学发光中的应用研究

林瑜, 谭学才*(), 吴叶宇, 韦富存, 吴佳雯, 欧盼盼   

  1. 广西民族大学化学化工学院 林产化学与工程国家民委重点实验室 广西林产化学与工程重点实验室 广西林产化学与工程协同创新中心 广西高校食品安全与药物分析化学重点实验室 南宁 530008
  • 收稿日期:2021-04-01 修回日期:2021-06-26 出版日期:2021-07-29 发布日期:2021-07-29
  • 通讯作者: 谭学才
  • 基金资助:
    国家自然科学基金项目(21365004); 广西科技重大专项子课题(桂科 AA18118013-10); 广西重点研发计划项目(桂科 AB18126048); 广西科技基地和人才专项(AD18126005); 广西研究生教育创新计划项目(JGY2019062); 广西高等教育本科教学改革工程项目(2015JGA194); 2021年广西博士研究生创新项目(YCBZ2021060)
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Two-Dimensional Nanomaterial g-C3N4 in Application of Electrochemiluminescence

Yu Lin, Xuecai Tan(), Yeyu Wu, Fucun Wei, Jiawen Wu, Panpan Ou   

  1. School of Chemistry and Chemical Engineering, Guangxi Minzu University, Key Laboratory of Chemistry and Engineering of Forest Products, State Ethnic Affairs Commission, Guangxi Key Laboratory of Chemistry and Engineering of Forest Products, Guangxi Collaborative Innovation Center for Chemistry and Engineering of Forest Products, Key Laboratory of Guangxi Colleges and Universities for Food Safety and Pharmaceutical Analytical Chemistry, Nanning 530008, China
  • Received:2021-04-01 Revised:2021-06-26 Online:2021-07-29 Published:2021-07-29
  • Contact: Xuecai Tan
  • Supported by:
    National Natural Science Foundation of China(21365004); Sub-Project of Guangxi Science and Technology Major Project(AA18118013-10); Guangxi Key Research and Development Program(AB18126048); Guangxi Science and Technology Base and Talents Special Project(AD18126005); Guangxi Graduate Education Innovation Project(JGY2019062); Guangxi Higher Education Undergraduate Teaching Reform Project(2015JGA194); 2021 Guangxi Doctoral Innovation Project(YCBZ2021060)

电化学发光(ECL)兼备电化学和化学发光的特点,灵敏度高、线性范围宽、背景干扰小,得到了广大分析科学研究者的关注;传统的ECL材料虽然发光效率高,但仍存在价格昂贵、负载量低等缺点。g-C3N4是一种不含金属的半导体纳米材料,主要以三嗪环或七嗪环为基本结构单元,通过层间的范德华力以及层内的C—N共价键结合,构成类石墨的二维层状结构,具有性质稳定、能带结构独特、生物兼容性好、环保无毒、易于功能化、原料价廉、制备过程简单等优点。自2012年g-C3N4首次被发现具备ECL的性能,至今已被广泛应用到ECL中。本文根据ECL的发光机理、传感器的作用效果、传感的信号类型以及不同的检测对象进行了分类,综述了近年来g-C3N4在ECL传感器构建中的研究进展,并阐述了g-C3N4在ECL发展中存在的挑战和前景。

关键词： g-C3N4, 电化学发光, 传感器

Electrochemiluminescence (ECL) combines the characteristics of electrochemistry and chemiluminescence. Because of its high sensitivity, wide linear range and low background interference, electrochemiluminescence has attracted the attention of many researchers in analytical science. Although the traditional luminescent materials of ECL have high luminous efficiency, they still have some disadvantages, such as high price, lower sample load, etc. g-C3N4 is a kind of metal-free semiconductor nanomaterial, which is based on triazine ring or heptazine ring as the basic structural unit. g-C3N4 is a two-dimensional graphite-like layered structure bonded by vander Waals forces between layers and C—N covalent bonds within layers. Since g-C3N4 was first discovered to have ECL performance in 2012, it had been widely used in the development and fabrication of ECL sensors, due to its advantages, such as stable property, unique band structure, good biocompatibility, better environmental performance, easy to function, inexpensive ingredients and simple preparation process. The research progresses of g-C3N4 in ECL sensor construction in recent years were reviewed, according to the mechanism of ECL luminescence, the effect of sensor, the signal type of sensor,and the different types of detection objects. And the challenges and prospects of g-C3N4 in ECL development were described as well.

Contents

1 Introduction

2 Classification according to luminescence mechanism

2.1 ECL cathodic co-reactant

2.2 ECL anode co-reactant

2.3 Other co-reactant

3 Classification according to sensor effect

3.1 Enhanced ECL sensor

3.2 Quenching ECL sensor

3.3 ECL sensors for both enhancement and quenching

4 Classification according to the signal type of the ECL sensor

4.1 Single signal ECL sensor

4.2 Double signal ECL sensor

5 Classification according to the target

5.1 Ions and small molecules

5.2 Nucleic acid

5.3 Protein immune

6 Conclusion and outlook

Key words: g-C3N4, electrochemiluminescence, sensor
()
图1 (a) ECL在1964—2002年的发展历程[16]; (b) ECL在2002年至今的发展历程
Fig. 1 (a) The development process of ECL from 1964 to 2002[16]; (b) the development process of ECL from 2002 to present
图2 g-C3N4的两种基本结构单元: (a) 三嗪环(C3N3),(b) 七嗪环(C6N7)
Fig. 2 Two basic structural units of g-C3N4: (a) C3N3, (b) C6N7
图3 (a) 基于Ag-g-C3N4构建检测SCCA的增强型ECL传感器[49]; (b) 基于g-C3N4-CD-Fc-COOH增强型ECL传感器的构建[50]
Fig. 3 (a) The enhanced ECL sensor for SCCA detection based on Ag-g-C3N4[49]; (b) construction process of enhanced ECL sensor based on g-C3N4-CD-Fc-COOH[50]
图4 基于g-C3N4/APBA/PANI的猝灭型ECL传感器的构建[52]
Fig. 4 The construction of quenching ECL sensor based on g-C3N4/APBA/PANI[52]
图5 (a) 先增强后降低的ECL传感器的构建[55];(b) 先猝灭后增强的ECL传感器的构造[56];(c) 先增强后猝灭再增强的ECL传感器的构建[57]
Fig. 5 (a) Construction of ECL sensor which signal increased at the early stage and then decreased[55];(b) construction of ECL sensor which signal decreased at the early stage and then increased[56];(c) construction of ECL sensor which signal enhanced, quenched then increased respectively[57]
图6 基于C60/g-C3N4单信号ECL传感器的构建[60]
Fig. 6 Construction of single signal ECL sensor based on C60/g-C3N4[60]
图7 (a) 基于g-C3N4和Ru(bpy)32+的双波长比率型ECL传感器的构建[61];(b) 基于g-C3N4双电位比率型ECL传感器的构建[48]
Fig. 7 (a) Construction of dual wavelength ratio ECL sensor based on g-C3N4 and Ru(bpy)32+[61];(b) construction of double potential ratio ECL sensor based on g-C3N4[48]
表1 基于g-C3N4的电化学发光传感器在离子或小分子检测中的应用
Table 1 The application of electrochemiluminescence sensor based on g-C3N4 in ions or small molecules detection
Target Material Linear range Detection limit ref
Cu2+ g-C3N4 2.5~100 nmol/L 0.9 nmol/L 31
Cu2+ g-C3N4 42.45~115.54 μmol/L 6.96 μmol/L 65
Cu2+ C,N QDs@g-C3N4 NSs 5 × 10-4~10 μmol/L 2 × 10-4 μmol/L 66
Cu2+ g-C3N4 0~45 nmol/L 1.2 nmol/L 67
Cu2+ g-C3N4/GO 1.0 × 1~1.0 × 1 mol/L 1.0 × 10-11mol/L 68
Pb2+ g-C3N4 QDs@NPG 0.05~20 nmol/L 0.02 nmol/L 69
GSH g-C3N4 0~100 μmol/L 9.6 nmol/L 70
GSH g-C3N4/MnO2 0.2~100 μmol/L 0.05 μmol/L 71
dopamine g-C3N4/MWCNTs 4.0 × 10-10~3.0 × 10-7 mol/L 0.19 nmol/L 42
dopamine g-C3N4/PANI 0.10 pM~5.0 nmol/L 0.033 pmol/L 52
dopamine Ag-g-C3N4 0.015~150 μmol/L 0.005 μmol/L 72
glucose Au-g-C3N4 0.1~8000 μmol/L 0.05 μmol/L 73
dopamine Au NF@g-C3N4-PANI 5.0 × 10-9~1.6 × 10-6 mol/L 1.7 × 10-9 mol/L 74
dopamine g-C3N4-PTCA 6.0 pM~30.0 nmol/L 2.4 pmol/L 75
Pen Hb/Au-g-C3N4 1.0 × 10-4~5.0 × 10-3 mol/L 3.1 × 10-5 mol/L 76
folic acid g-C3N4-rGO 0.1~90 nmol/L 62 pmol/L 77
glucose Ppy/Plu/C3N4-Ni(OH)2/GOx 0.5~500 μmol/L 0.04 μmol/L 78
diclofenac GO-g-C3N4/MWCNTs-AuNPs 0.005~1000 ng/mL 1.7 pg/mL 49
gibberellin Au-g-C3N4 4.0 × 10-14~7.0 × 10-11mol/L 1.64 × 10-14mol/L 79
gatifloxacin rGO-CuS-g-C3N4 1.0 × 10-4~1.0 × 10-8 mol/L 3.5 × 10-9 mol/L 80
adrenaline g-C3N4 /MWCNTs 1.0 × 10-9~1.5 × 10-6 mol/L 0.21 nmol/L 81
riboflavin g-CN QDs 0.02~11 μmol/L 0.63 nmol/L 82
Cu2+ g-C3N4 NSs/GQDs 5.5 × 10-10~4.5 × 10-6 mol/L 3.7 × 10-10 mol/L 83
PFOA MIP@utg-C3N4 0.02~40.0 ng/mL 0.01 ng/mL 84
BPA C-g-C3N4 0.1 pM~1 nmol/L 30 fmol/L 85
fipronil ZnO@g-C3N4 5~1000 nmol/L 1.5 nmol/L 86
Aflatoxin g-C3N4 0.005~10 ng/mL 0.004 ng/mL 87
图8 基于g-C3N4的ECL基因检测传感器的构建[88]
Fig. 8 Construction of ECL gene detection sensor based on g-C3N4[88]
表2 基于g-C3N4的ECL传感器在蛋白免疫的应用
Table 2 The application of electrochemiluminescence immunosensor based on g-C3N4
Target Material Linear range Detection limit ref
PDGF-BB β-CD/g-C3N4 /Fc 5 × 10-13~5 × 10-7 g/mL 2.6 × 10-13g/mL 91
PDGF-BB g-C3N4 QD@g-C3N4 NHs 0.02~80 nmol/L 0.013 nmol/L 57
CEA g-C3N4/ATA 0.1 pg/mL~1 ng/mL 3 fg/mL 92
CEA Au-g-C3N4 0.02~80 ng/mL 6.8 pg/mL 93
CEA g-C3N4 0.01 pg/mL~1 ng/mL 3 fg/mL 40
CEA Ag@g-C3N4 1 pg/mL~100 ng/mL 0.35 pg/mL 94
SCCA g-C3N4-graphene 0.025~10 ng/mL 8.53 pg/mL 95
Con A Ag-g-C3N4/PANI-PTCA-DexP 0.001~50 ng/mL 0.0003 ng/mL 96
Con A g-C3N4-COOH@Glu 1 × 10-5~1 × 104 ng/mL 2.2 fg/mL 58
Con A 3D-GR-Au NPs/DexP-g-C3N4 0.05~100 ng/mL 17 pg/mL 97
AFP Au-g-C3N4 0.1 pg/mL~1 ng/mL 0.03 pg/mL 40
AFP g-C3N4-CNTs 0.3 fg/mL~0.01 ng/mL 0.1 fg/mL 98
galactosyltransferase g-C3N4-PS 5 × 10-4~0.05 U/mL 7 × 10-5 U/mL 99
Amyloid β protein g-C3N4/Ru@MOF 10-5~500 ng/mL 3.9 fg/mL 62
Amyloid β protein g-C3N4-Heme 1.0 × 10-14~1.0 × 10-7 mol/L 3.2 × 10-15mol/L 100
AChE Au-g-C3N4 0.1 pg/mL~10 ng/mL 42.3 fg/mL 44
insulin AuPtAg@HP-g-C3N4 0.05 pg/mL~100 ng/mL 17 fg/mL 101
PSA Au@g-C3N4/Ru(bpy 0.10~200 ng/mL — 102
PSA g-C3N4@Cu2O 1.0 × 10-2~120 ng/mL 3.42 × 10-3 ng/mL 103
CA125 Fe3O4/g-C3N4 0.001~5 U/mL 0.4 mU/mL 104
CA125 g-C3N4-CdTe/CdS QDs 0.0001~10 U/mL 3.4 × 10-5 U/mL 105
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