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. 2025 Feb 11;18(4):796.
doi: 10.3390/ma18040796.

High-Level Lanthanide-Doped Upconversion Nanoparticles-Based Aptasensor to Increase Carcinoembryonic Antigen Detection Sensitivity

Lujun Niu  1 , Qiren Sun  1 , Shijia Wei  1 , Dixiang Gong  2 , Enhui Wang  1   3 , Yan Chen  1 , Lu Xia  4 , Xingyu Liu  4 , Langping Tu  5 , Long Shao  5 , Hongfei Li  5 , Jing Zuo  1
Affiliations

High-Level Lanthanide-Doped Upconversion Nanoparticles-Based Aptasensor to Increase Carcinoembryonic Antigen Detection Sensitivity

Lujun Niu et al. Materials (Basel). .

Abstract

Boosting the accuracy and speed of cancer detection is highly desirous in tumor detection, and sensors capable of detecting carcinoembryonic antigen (CEA) have great application prospects in this field. A highly sensitive sensor is constructed based on the fluorescence resonance energy transfer (FRET) with heavily rare-earth-doped upconversion nanoparticles (UCNPs) as energy donors and polydopamine nanoparticles (PDA NPs) as energy acceptors. This sensor detects the fluctuations in CEA molecules via luminescence quenching and recovery resulting from a competitive binding assay between CEA and PDA NPs. The high-level-doped design of UCNPs (i.e., NaYF4@NaYbF4:1%Tm@NaYF4) is beneficial, providing upconversion luminescence intensity that is more than 10 times higher than that of the conventional low-level-doped UCNPs (i.e., NaYF4@NaYF4:20%Yb, 0.2%Tm@NaYF4). The sensor exhibits impressive sensitivity. Specifically, in diluted fetal bovine serum, the detection limit reaches 0.013 ng/mL in the range of 0-1.5 ng/mL (S/N = 3), while the detection limit is 1.38 ng/mL in the range of 1.5-250 ng/mL (S/N = 3). This method has great potential for future applications in the rapid and early diagnosis and treatment of cancer.

Keywords: CEA detection; FRET; UCNPs-PDA NP sensor; high-level doping.

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Conflict of interest statement

Authors Lu Xia and Xingyu Liu are employed by the company The 49th Research Institute of China Electronics Technology Group Corporation. The remaining authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.

Figures

Figure 1
Figure 1
A schematic illustration of the formation of a biosensor for detecting carcinoembryonic antigen (CEA) based on upconversion nanoparticles (UCNPs)-polydopamine nanoparticles (PDA NPs): (a) the synthesis process of NaYF4@NaYF4:Yb,Tm@NaYF4 core–shell–shell UCNPs; (b) the construction of the UCNP and CEA aptamer combination; (c) polydopamine synthesis; (d) the fluorescence quenching and fluorescence recovery processes of the detecting system.
Figure 2
Figure 2
Characterization of synthesized nanoparticles: (a) HAADF-STEM image of NaYF4@NaYbF4:1%Tm@NaYF4 core–shell–shell nanoparticles; (b) scanning TEM image and element mappings of Tm, Yb, Y, and Na, with an overlap of Y, Tm, and Yb for the sample in panel a; (c) the particle size distribution of the sample in panel a; (d) high-resolution TEM image of one NaYF4@NaYbF4:1%Tm@NaYF4 core–shell–shell nanoparticle; (e) XRD image of NaYF4@NaYbF4:1%Tm@NaYF4 and the standard card (JCDSP No. 16-0334).
Figure 3
Figure 3
(a) FTIR spectra of NaYF4@NaYbF4:1%Tm@NaYF4 (without an organic layer, bule line), and NaYF4@NaYbF4:1%Tm@NaYF4-CEA aptamer (green line); (b) UV–vis absorption spectra of NaYF4@NaYbF4:1%Tm@NaYF4 and NaYF4@NaYbF4:1%Tm@NaYF4-CEA aptamer; (c) FTIR spectra of dopamine and PDA NPs; (d) absorption spectra of PDA NPs, and emission spectra of NaYF4@NaYbF4:1%Tm@NaYF4 UCNPs.
Figure 4
Figure 4
(a) Fluorescence quenching of NaYF4@NaYbF4:1%Tm@NaYF4-CEA aptamer system with different concentrations of PDA NPs (the reaction time was fixed at 20 min); (b) reaction-time-dependent fluorescence quenching of NaYF4@NaYbF4:1%Tm@NaYF4-CEA aptamer-PDA system (the concentration of PDA NPs was fixed at 0.35 μg/μL).
Figure 5
Figure 5
(a) Fluorescence recovery of Y@99Yb1Tm@Y-CEA aptamer-PDA NP system with different CEA concentrations; (b) fluorescence recovery of Y@20Yb0.2Tm@Y-CEA aptamer-PDA NP system with different CEA concentrations; (c) steady-state emission spectra of two types of UCNP under 980 nm laser irradiation (0.80 W cm−2); (d) relative fluorescence intensity of sensor (0.01 mg/mL) in presence of Gly (1.0 μg/mL), L-AscH2 (1.0 μg/mL), L-Cys (1.0 μg/mL), Glu (1.0 μg/mL), BSA (1.0 μg/mL), NaCl (1.0 μg/mL), and CEA (50 ng/mL). Experiments were performed in HEPES buffer (10 mM, pH 7.4).
Figure 6
Figure 6
Fluorescence recovery of Y@99Yb1Tm@Y-CEA aptamer-PDA NPs system with different CEA concentrations in diluted fetal bovine serum.
See this image and copyright information in PMC

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