稀土发光材料在免疫分析中的应用研究进展

doi:10.19894/j.issn.1000-0518.250259

摘要/Abstract

摘要：

稀土发光材料是以稀土元素为发光中心的一类发光材料，其凭借窄带发射、长的荧光寿命和大的Stokes位移等独特的光物理特性在照明、显示、激光、生物医学、防伪和光通信等众多领域展现出巨大的应用潜力。本文总结了稀土元素的特性、发光材料的种类与原理，并基于不同稀土材料在时间分辨荧光检测、近红外二区荧光检测和上转换荧光检测等技术中的应用，系统综述了稀土发光材料在免疫分析领域的应用，最后对其在临床实际应用中面临的挑战与未来发展方向进行了展望。

关键词: 稀土发光材料, 时间分辨荧光, 免疫分析, 生物传感器

Abstract:

Rare earth （RE） luminescent materials， leveraging unique optical properties such as long fluorescence lifetimes， large Stokes shifts， and narrow-band emissions， have become pivotal for high-sensitivity immunoassays. Rare earth luminescent materials can be broadly classified into the following categories： 1） organic coordination compound-based rare earth luminescent materials， 2） inorganic matrix-doped rare earth luminescent materials， and 3） upconversion nanoluminescent materials. This article systematically reviews the properties of rare earth elements， the types and principles of luminescent materials. Based on three biometric detection techniques， namely time-resolved fluorescence detection， near-infrared （NIR-Ⅱ） fluorescence detection， and upconversion fluorescence detection， it delves into the applications of rare earth luminescent materials in the field of immunoassay. Finally， it discusses the challenges these materials face in clinical applications and prospects for future development.

Key words: Rare earth luminescent materials, Time-resolved fluorescence, Immunoassay, Biosensors

中图分类号:

O613

戴斌, 彭琳, 朱雪宁, 王特, 杨赛男, 张玲玲. 稀土发光材料在免疫分析中的应用研究进展[J]. 应用化学, 2025, 42(8): 1057-1069.

Bin DAI, Lin PENG, Xue-Ning ZHU, Te WANG, Sai-Nan YANG, Ling-Ling ZHANG. Research Progress on the Application of Rare Earth Luminescent Materials in Immunoassay[J]. Chinese Journal of Applied Chemistry, 2025, 42(8): 1057-1069.

图/表 8

图1 稀土发光材料的种类以及应用领域［41-42］

Fig.1 Types and application fields of rare earth luminescent materials［41-42］

表1 稀土发光化合物在时间分辨荧光分析中的应用

Table 1 Application of rare earth luminescent compounds in time resolved fluorescence detection

Rare earth compound	Analysis technique	Target	Linear range/（ng·mL^-1）	LOD/（ng·mL^-1）	Ref.
Eu chelates	Time-resolved fluorescence immunoassay	African swine fever virus	0.24~5	0.015	［44］
Sm chelates	Time-resolved fluorescence immunoassay	Lipoprotein（a）	0~5	0.000 64	［45］
Eu chelates	Time-resolved fluorescence immunoassay	Aflatoxin B1	0.1~3.94	0.1	［46］
Eu cryptate	Homogenous time-resolved fluorescence	Bacterial protective antigen	2~2 500	2	［47］
LiLuF₄∶Ce/Tb NPs	Time-resolved fluorescence resonance energy transfer	Biotin	0~152 600	210	［48］
Eu chelate	Time-resolved fluorescence resonance energy transfer	Cardiac troponin I	0~1.16	0.097	［49］
Eu chelate	AlphaLISA	Staphylococcal enterotoxin B	0.025~25	0.025	［50］

图2 基于免疫磁珠的时间分辨荧光免疫分析法（TRFIA）检测癌胚抗原示意图［54］

Fig.2 Schematic diagram of carcinoembryonic antigen detection by time-resovlved fluoroimmunoassay （TRFIA） based on immunomagnetic beads［54］

图3 （A）游离生物素与链酶亲和素示意图；（B） TR-FRET法定量测定生物素原理图，当游离生物素存在时，APC标记的生物素结合概率降低，产生较弱的665 nm荧光强度和较强的620 nm荧光强度；（C）荧光信号随生物素浓度的变化曲线图［59］；（D） ADP传感器原理图，当存在游离ADP时，Tb标记抗体的ADP与QD的FRET过程减弱；（E） ADP传感器的荧光团的光谱［60］

Fig.3 （A） Schematic diagram of the binding of free biotin and streptavidin；（B） Schematic diagrams of the principle for quantitative determination of biotin by TR-FRET. In the presence of free biotin， the binding probability of APC-labeled biotin decreases， resulting in weaker fluorescence intensity at 665 nm and stronger fluorescence intensity at 620 nm；（C） Curve diagram of the changes in fluorescence signal with biotin concentration［59］；（D） Schematic diagram of the ADP sensor： in the presence of free ADP， the FRET process between Tb-labeled antibody-bound ADP and QDs is weakened；（E） Spectra of the fluorophores of the ADP sensor［60］

图4 （A）光引发化学发光检测技术原理图：只有在免疫过程发生时，680 nm激光激发后，通过单线态氧的共振能量转移，该体系才可发射610 nm的荧光；（B）基于光引发化学发光检测技术的CRP浓度与化学发光信号关系图；（C）基于光引发化学发光检测技术的IFN-γ浓度与化学发光信号关系图；（D）基于光引发化学发光检测技术的PCT浓度与化学发光信号关系图［66］；（E） GM的光激化学发光测定示意图［67］

Fig.4 （A） Schematic diagram of the principle of light-initiated chemiluminescent assay technology；（B） Graph showing the relationship between CRP concentration and chemiluminescence signal based on light-initiated chemiluminescent assay technology；（C） Graph showing the relationship between IFN-γ concentration and chemiluminescence signal based on light-initiated chemiluminescent assay technology；（D） Graph showing the relationship between PCT concentration and chemiluminescence signal based on light-initiated chemiluminescent assay technology［66］；（E） Schematic diagram of light-initiated chemiluminescent assay of GM［67］

图5 （A）量子点对微球编码流程图；（B）多重LOCI技术用于多重检测的原理示意图［73］

Fig.5 （A） Flow chart of microsphere encoding by quantum dots；（B） Schematic diagram of the principle of multi-LOCI technology for multiplex detection［73］

图6 （A） LFA平台中不同种类荧光探针的信噪比垂直剖面图；（B） NaYF4∶7%Nd@NaYF4纳米粒子结构图［78］；（C） 980 nm激发下1550 nm发射度的Yb， Er/Ce共掺杂纳米粒子结构图；（D）基于NIR-II发射Yb， Er/Ce共掺杂纳米粒子的横向流动免疫分析平台示意图［79］

Fig.6 （A） Vertical cross-sectional view of the signal-to-noise ratio of different types of fluorescent probes in the LFA platform；（B） Structural diagram of NaYF4∶7%Nd@NaYF4 nanoparticles［78］；（C） Structural diagram of Yb，Er/Ce co-doped nanoparticles with 1550 nm emission under 980 nm excitation；（D） Schematic diagram of the lateral flow immunoassay platform based on NIR-Ⅱ emitting Yb，Er/Ce co-doped nanoparticles［79］

图7 （A）稀土上转换纳米探针的构建及其基于发光共振能量传递技术的CA125传感示意图［82］；（B） miRNA-21检测示意图［83］

Fig.7 （A） Schematic illustration of the construction of rare earth upconversion nanoprobes and the CA125 sensing based on luminescence resonance energy transfer technology［82］；（B） Schematic diagram of miRNA-21 detection［83］

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