用于丝网印刷光电化学生物传感器的功能纳米材料的最新进展

doi:10.3866/PKU.WHXB202310046

物理化学学报 >> 2025, Vol. 41 >> Issue (2): 100018.doi: 10.3866/PKU.WHXB202310046

所属专题：新型光电功能材料

综述上一篇

用于丝网印刷光电化学生物传感器的功能纳米材料的最新进展

杨美清¹, 王路², 卢浩滋², 杨耀成³^,*(), 刘松²^,*()

¹ 湖南文理学院生命与环境科学学院, 湖南省动物学重点实验室, 湖南常德 415000
² 湖南大学化学化工学院, 化学生物传感与计量学国家重点实验室, 化学生物学与纳米医学研究所, 长沙 410082
³ 中南大学湘雅二医院骨科, 长沙 410011

收稿日期:2023-10-31 修回日期:2023-11-29 录用日期:2023-11-30 发布日期:2024-01-09
通讯作者: Email: yangyaocheng@csu.edu.cn (杨耀成)liusong@hnu.edu.cn (刘松)
基金资助:
湖南文理学院博士科研启动基金(21BSQD43); 湖南省自然科学基金(2023JJ40463); 国家自然科学基金(22175060)

Recent Advances of Functional Nanomaterials for Screen-Printed Photoelectrochemical Biosensors

Yang Meiqing¹, Lu Wang², Haozi Lu², Yaocheng Yang³^,*(), Song Liu²^,*()

¹ Zoology Key Laboratory of Hunan Higher Education, College of Life and Environmental Science, Hunan University of Arts and Science, Changde 415000, Hunan Province, China
² Institute of Chemical Biology and Nanomedicine (ICBN), State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China
³ Department of Orthopaedics, The Second Xiangya Hospital, Central South University, Changsha 410011, China

Received:2023-10-31 Revised:2023-11-29 Accepted:2023-11-30 Published:2024-01-09
Contact: Email: yangyaocheng@csu.edu.cn (Yaocheng Yang)liusong@hnu.edu.cn (Song Liu)
Supported by:
the Doctoral Research Start-up Fund of Hunan University of Arts and Science(21BSQD43); the Natural Science Foundation of Hunan Province, China(2023JJ40463); the National Natural Science Foundation of China(22175060)

摘要/Abstract

摘要：

光电化学(PEC)生物传感器因其低背景、高灵敏度、高特异性和快响应速度等优点而备受关注。近年来，一次性丝网印刷电极(SPE)的引入极大地推动了PEC生物传感器的发展，使丝网印刷PEC生物传感器成为一种应用前景广阔的分析工具。在丝网印刷PEC生物传感器的构建过程中，光活性纳米材料起着至关重要的作用，因为它们不仅可用作光电转换平台，还可用作生物识别元件的装载平台。然而，单纯的光活性材料通常存在一些缺点，比如固有的毒性、宽带隙、高的电子空穴对重组率等，因此，通过各种设计策略来改善光活性材料的光电特性是十分必要的。为了获得高灵敏度的丝网印刷PEC生物传感器，通常还需要将高性能光电极与各种信号放大策略相结合。鉴于此，我们在本文中首次对用于丝网印刷PEC生物传感器的光活性材料进行了系统总结，并将其归为四大类：金属氧化物、金属硫族化合物、碳纳米材料和铋基纳米材料。同时，我们重点关注了光活性材料的设计策略，例如形态调控、元素掺杂、异质结构建等。此外，我们还通过具有代表性的丝网印刷PEC免疫传感器和丝网印刷PEC适体传感器介绍了一些信号放大策略，如酶标记放大(ELA)策略、聚合酶链反应(PCR)策略、滚环扩增(RCA)策略和杂交链式反应(HCR)策略。最后，我们还讨论了丝网印刷PEC生物传感器目前面临的挑战和前景。我们希望通过本文让读者全面了解丝网印刷PEC生物传感器的最新进展，并为该领域的未来发展提供可行性指导。

关键词: 光电化学分析, 生物传感器, 丝网印刷电极, 光活性材料, 信号放大技术

Abstract:

Photoelectrochemical (PEC) biosensors have attracted intensive attention due to their advantages, including low background, high sensitivity, high specificity and rapid response. In recent years, the introduction of disposable screen-printed electrodes (SPE) has greatly facilitated the development of PEC biosensors, making screen-printed PEC biosensors a promising analytical tool for various applications. Photoactive nanomaterials play a crucial role in the construction of screen-printed PEC biosensors as they can be used not only as photoelectric conversion platforms but also as loading platforms for recognition elements. However, pure photoactive materials usually suffer from some drawbacks, such as inherent toxicity, wide bandgap, and high electron-hole pair recombination rate. Therefore, it is necessary to improve the photoelectric properties of these materials through various design strategies. Moreover, to obtain highly sensitive screen-printed PEC biosensors, it is usually necessary to combine the high-performance photoelectrodes with various signal amplification strategies. In view of this, we provide the first systematic summary of photoactive materials for screen-printed PEC biosensors in this paper, classifying them into four main categories: metal oxides, metal chalcogenides, carbon nanomaterials and bismuth-based nanomaterials. Meanwhile, we focus on the design strategies for photoactive materials, including morphology modulation, elemental doping, and heterostructure construction. In addition, we introduce signal amplification strategies, such as the enzyme label amplification (ELA) strategy, polymerase chain reaction (PCR) strategy, rolling circle amplification (RCA) strategy, and hybridization chain reaction (HCR) strategy, through representative screen-printed PEC immunosensors and screen-printed PEC aptasensors. Finally, we discuss the current challenges and prospects of screen-printed PEC biosensors. We hope to provide readers with a comprehensive understanding of the recent advances in screen-printed PEC biosensors and provide a feasible guidance for the future development of this field.

Key words: Photoelectrochemical analysis, Biosensor, Screen-printed electrode, Photoactive materials, Signal amplification technique

杨美清, 王路, 卢浩滋, 杨耀成, 刘松. 用于丝网印刷光电化学生物传感器的功能纳米材料的最新进展[J]. 物理化学学报, 2025, 41(2), 100018. doi: 10.3866/PKU.WHXB202310046

Yang Meiqing, Lu Wang, Haozi Lu, Yaocheng Yang, Song Liu. Recent Advances of Functional Nanomaterials for Screen-Printed Photoelectrochemical Biosensors[J]. Acta Phys. -Chim. Sin. 2025, 41(2), 100018. doi: 10.3866/PKU.WHXB202310046

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202310046

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I2/100018

图/表 11

图1

图2

表1

Electrode	Photoactive material	Recognition element	Target	Limit of detection	Linear range	Ref.
CdS/ZnO/PDDA-CNTs/PWE	CdS QD/ZnO spheres	antibody	CEA	4 pg∙mL⁻¹	0.01 to 50 ng·mL⁻¹	36
CdS/ZnO/Au@Pt-PWE	CdS QD/ZnO nanorods	antibody	CEA; AFP	CEA: 0.3 pg·mL⁻¹; AFP: 0.5 pg·mL⁻¹	1.0 pg·mL⁻¹ to 100 ng·mL⁻¹	37
ZnO/Au PWE	CdS nanorods/ ZnO spheres	antibody	PSA	2.3 pg·mL⁻¹	0.005 to 150 ng·mL⁻¹	38
CdS/ZnO/rGO-PWE	CdS QDs/ZnO nanorods	antibody	CA 125	2.0 × 10⁻⁴ U·mL⁻¹	5.0 × 10⁻⁴ U·mL⁻¹ to 500 U·mL⁻¹	39
CdS/ZnO/rGO/cellulose	CdS QDs/leaf-shape ZnO	capture DNA	adenosine; potassium ion	adenosine: 0.15 nM ^*; potassium ion: 0.06 nM	adenosine: 0.5 nM to 50 μM; potassium ion: 0.1 nM to 50 μM	40
CdS/ZnO/PAE	CdS QDs/ZnO nanotubes	aptamer	PSA	0.34 pg·mL⁻¹	0.001 to 80 ng·mL⁻¹	41
CdS/rGO/ZnO/Au-PWE	CdS QDs/rGO/ ZnO nanorods	hairpin DNA	miRNA-21; miRNA-122b; miRNA-7f	miRNA-21: 0.32 fM; miRNA-122b: 0.37 fM; miRNA-7f: 3.8 fM	miRNA-21: 0.5 fM to 100 pM; miRNA-122b: 0.5 fM to 100 pM; miRNA-7f: 10 fM to 100 pM	42
CdSe/ZnO/Au/SPCE	CdSe QDs/ZnO networks	aptamer	ATP	6.3 nM	10 nM to 3 μM	43
CdTe/ZnO/Au-PWE	CdTe QDs/ZnO spheres	aptamer	MCF-7 cell	21 cells·mL⁻¹	63–1.0 × 10⁷ cell·mL⁻¹	44
ZnO/CuInS₂/PAE	ZnO nanoflakes/ CuInS₂/Ag₂Se QDs	hairpin DNA	miRNA-141	16.7 fM	50 fM to 100 pM	45
Au/ZnO/graphene/ITO	ZnO naospheres/graphene	aptamer	SK-BR-3 breast cancer cell	58 cells·mL⁻¹	1 × 10²−1 × 10⁶ cells·mL⁻¹	46
N-Cdots/ZnO/ Au@3D-rGO/cellulose	N-Cdots/astroid ZnO	aptamer	thrombin	16.7 fM	50 fM to 1000 pM	47
GQDs/ZnO/Au	ZnO nanorods/GQDs/Ag₂Se QDs	aptamer	MCF-7 cell	198 cells·mL⁻¹	5.0 × 10² to 5.0 × 10⁶ cells·mL⁻¹	48
Ag₂Se/GQDs/ZnO/Au-PWE	Ag₂Se/GQDs/ZnO nanosheets	DNA	miRNA-141	52 aM	0.15 fM to 2 nM	49
ZnNc-COOH/ZnO/Au-PWE	ZnNc-COOH/ZnO nanorods	antibody	CEA	1.6 pg·mL⁻¹	0.005–100 ng·mL⁻¹	50
AuNPs/CS/TiO₂-graphene/CS/SPCE	TiO₂ nanobelts-graphene	antibody	CEA	0.28 pg·mL⁻¹	0.5–8000 pg·mL⁻¹	51
Amb/Ni_x-gC₃N₄/TiO₂/SPCE	Amb/Ni_x-gC₃N₄/TiO₂ nanoparticles	antibody	PSA	0.06 fg·mL⁻¹	10⁻¹⁶–10⁻⁸ g·mL⁻¹	52
N-Cdots/TiO₂-Pt/PWE	N-Cdots/TiO₂ nanoparticle	aptamer	CEA	1.0 pg·mL⁻¹	0.002–200 ng·mL⁻¹	53
N-Cdots/TiO₂/Pt/PWE	N-Cdots/TiO₂ nanotubes	primer strand	CEA	0.48 pg·mL⁻¹	0.001–200 ng·mL⁻¹	54
CdS/TiO₂/Au-PWE	CdS/TiO₂	antibody	CEA	0.065 pg·mL⁻¹	0.1 pg·mL⁻¹–5 μg·mL⁻¹	55
cellulose paper/PSATs/CdS	PSATs/CdS	ssDNA	cTnI	0.47 fg·mL⁻¹	1.2 fg·mL⁻¹–20 ng·mL⁻¹	56
TiO₂@Au/ITO	TiO₂@Au/CdS Z-scheme structure	ssDNA	nine HPV genotyping	0.1 copies·μL⁻¹	0.6–600 copies·μL⁻¹	57
TiO₂/MIL-125-NH₂/Au-PWE	TiO₂/MIL-125-NH₂	DNA	miRNA-182-5p	0.09 fM	10^–16 to 10^–10 M	58
CuO/rGO/cellulose	CuO nanoflowers	aptamer	ATP	2.1 nM	5.0 to 3.0 × 10³ nM	59
Bi₂S₃-BiVO₄/Cu₂O/PAE	BiVO₄-Bi₂S₃/Cu₂O	hairpin DNA	miRNA-141	0.17 fM	0.5 fM to 5 nM	60
BiVO₄/Cu₂O/rGO-PWE	BiVO₄/Cu₂O	DNA	miRNA-141	83 aM	0.25 fM to 1 nM	61
Au-PWE/FeOOH/Cu₂O/CuS	FeOOH/Cu₂O/CuS	DNA	miRNA-141	0.11 fM	0.3 fM to 10 nM	62
WO₃/SPE	flower-like WO₃	antibody	okadaic acid	0.007 ng·mL⁻¹	0.01–60 ng·mL⁻¹	63
WO₃/Fe₂O₃/Au-PWE	WO₃/Fe₂O₃	aptamer	mucin 1; miRNA-21	mucin 1: 3.4 fg·mL⁻¹; miRNA-21: 36 fM	mucin 1: 10 fg·mL⁻¹–100 ng·mL⁻¹; miRNA-21: 0.1 pM–10 nM	64
In₂S₃-P/WO₃/Au-PWE	In₂S₃-P/WO₃	aptamer	OTA	0.052 pg·mL⁻¹	10⁻¹³ to 10⁻⁷ g·mL⁻¹	65
SnO₂ QD/rGO/Au-PWE	SnO₂ QD/rGO	ssDNA	ATP	0.025 pM	0.1 pM to 100 nM	66
Sn-self doped SnO_2−x/Au-PWE	Sn-self doped SnO_2−x nanotubes	antibody	AFP	3.84 pg·mL⁻¹	10 pg·mL⁻¹ to 200 ng·mL⁻¹	67
CeO₂-PTNs	CeO₂-PTNs heterostructure	hairpin DNA	thrombin	6.7 fM	0.02 pM to 100 pM	68
CQDs-MnO₂/SPCE	CQDs-MnO₂ heterojunctions	antibody	AFP	9.3 pg·mL⁻¹	0.01 to 100 ng·mL⁻¹	69
In₂O₃-In₂S₃/SPE	In₂O₃-In₂S₃	Cas12a-CrRNA	HPV-16	1.2 pM	5.0 to 5000 pM	70

表1

图3

图4

图5

表2

图6

图7

图8

图9

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Electrode	Photoactive material	Recognition element	Target	Limit of detection	Linear range	Ref.
CdS/PDDA-CNTs/PWE	CdS NPs	antibody	CEA	2.1 pg·mL⁻¹	0.01 to 50 ng·mL⁻¹	73
CdS/PDDA-CNTs/PWE	CdS NPs	aptamer	ATP	0.2 pM	1.0 pM to 1.0 nM	74
CdS/PDDA-GR/ Au-PWE	CdS NPs	ssDNA	DNA	15 fM	50.0 fM to 100 nM	75
CdS/SPCE	CdS QDs	antibody	HSA	1.97 ng·mL⁻¹	0 to 100 ng·mL⁻¹	76
CdS-Fe₃O₄/SPE	CdS QDs-Fe₃O₄	antibody	AFB₁	5.0 pg·mL⁻¹	0.01 to 80 ng·mL⁻¹	77
Au/SPCE	Au/PANI@CdS	antibody	Cyfra 21-1	0.035 pg·mL⁻¹	0.1 pg·mL⁻¹ – 100 ng·mL⁻¹	78
CdS@CdMoO₄/ SPE	hollow CdS/CdMoO₄ heterostructures	antibody	CEA	11.3 pg·mL⁻¹	0.02 to 50.0 ng·mL⁻¹	79
EGNPs/CdTe-GO/SPE	CdTe QDs-GO	aptamer	17β-estradiol	0.01 pM	0.04 to 10 pM	80
Au/SPE	SnSe QD	antibody	CA19-9	0.0011 U·mL⁻¹	0.005–100 U·mL⁻¹	81
MSPPE	rGO-MoS₂ sheets	antibody	Escherichia coli O157:H7	2.0 CFU·mL⁻¹	5.0 – 5.0 × 10⁶ CFU·mL⁻¹	82
ZnIn₂S₄/SPE	ZnIn₂S₄	antibody	AFP	0.01 ng·mL⁻¹	0.05 to 1 ng·mL⁻¹ and 5 to 100 ng·mL⁻¹	83
Co₉S₈@ZnIn₂S₄/ SPE	Co₉S₈@ZnIn₂S₄ heterostructures	antibody	HER2	3.5 pg·mL⁻¹	0.01 to 10 ng·mL⁻¹	84
CuInS₂/CoIn₂S₄/ Au-WE	CuInS₂/CoIn₂S₄	hairpin DNA	miRNA-141	0.29 pM	0.5 pM to 2 nM	85

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用于丝网印刷光电化学生物传感器的功能纳米材料的最新进展

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