Core–Shell Interface Engineering Strategies for Modulating Energy Transfer in Rare Earth-Doped Nanoparticles
<p>(<b>a</b>,<b>b</b>) depict the synthesis of RENPs using the LBL strategy, while (<b>c</b>) illustrates simplified energy-level diagrams showing the energy transfer between Nd<sup>3+</sup>, Yb<sup>3+</sup>, and Er<sup>3+</sup> ions upon 808 nm excitation. (<b>d</b>,<b>e</b>) illustrate the energy transfer between rare earth ions in RENPs-LBL and RENPs-SA, respectively.</p> "> Figure 2
<p>Characterization of the as-synthesized core–shell Tm-RENPs. TEM image of as-synthesized Tm-RENPs-LBL: (<b>a</b>) core, (<b>b</b>) core@shell; Tm-RENPs-SA: (<b>e</b>) core, (<b>f</b>) core@shell; Er-RENPs-LBL: (<b>i</b>) core, (<b>j</b>) core@shell; Er-RENPs-SA: (<b>m</b>) core, (<b>n</b>) core@shell. HAADF-STEM images of (<b>c</b>) Tm-RENPs-LBL, (<b>g</b>) Tm-RENPs-SA, (<b>k</b>) Er-RENPs-LBL, and (<b>o</b>) Er-RENPs-SA. Chemical concentration profiles of (<b>d</b>) Tm-RENPs-LBL, (<b>h</b>) Tm-RENPs-SA, (<b>l</b>) Er-RENPs-LBL, and (<b>p</b>) Er-RENPs-SA. The concentration profiles were obtained from the EDXS line; white arrows indicate the EDXS scan direction.</p> "> Figure 3
<p>Characterization of the as-synthesized core–shell–shell Ce-RENPs. TEM image of as-synthesized Ce-RENPs-LBL (<b>a</b>) core; (<b>b</b>) core@shell 1; (<b>c</b>) core@shell 1@shell 2. TEM image of Ce-RENPs-SA: (<b>d</b>) core; (<b>e</b>) core@shell 1; (<b>f</b>) core@shell 1@shell 2. (<b>g</b>) XRD patterns of Ce-RENPs-LBL and Ce-RENPs-SA. Energy transfer diagram of (<b>h</b>) Ce-RENPs-LBL and (<b>k</b>) Ce-RENPs-SA. HAADF-STEM images of (<b>i</b>) Ce-RENPs-LBL and (<b>l</b>) Ce-RENPs-SA. Chemical concentration profiles of (<b>j</b>) Ce-RENPs-LBL and (<b>m</b>) Ce-RENPs-SA. The concentration profiles were obtained from the EDXS line; white arrows indicate the EDXS scan direction.</p> "> Figure 4
<p>Fluorescence spectra of Tm-RENPs synthesized by two strategies under (<b>a</b>) 980 nm laser excitation and (<b>b</b>) 808 nm laser excitation. Fluorescence spectra of Er-RENPs synthesized by two strategies under (<b>c</b>) 980 nm laser excitation and (<b>d</b>) 808 nm laser excitation. The red shaded part is the DSL spectrum detected by the NIR detector.</p> "> Figure 5
<p>Fluorescence spectra of Ce-RENPs synthesized by two strategies under (<b>a</b>) 808 nm and (<b>b</b>) 980 nm excitation in cyclohexane at a power density of 10.0 W cm<sup>−2</sup>. The red shaded part is the DSL spectrum detected by the NIR detector.</p> "> Figure 6
<p>DSL spectra of (<b>a</b>) Ce-RENPs-SA and (<b>b</b>) Ce-RENPs-LBL at 808 nm excitation. (<b>c</b>) The intensity ratio of 1060 nm emission to 980 nm emission of Ce-RENPs-SA and Ce-RENPs-LBL under 808 nm laser excitation varies with the thickness of shell 1. UCL spectra of (<b>d</b>) Ce-RENPs-SA and (<b>e</b>) Ce-RENPs-LBL at 980 nm excitation. (<b>f</b>) The intensity of 540 nm emission of Ce-RENPs-SA and Ce-RENPs-LBL under 980 nm laser excitation varies with the thickness of shell 1. The blue arrow shows that the fluorescence intensity increases with the increase of shell 1 thickness, and the green arrow vice versa.</p> "> Figure 7
<p>(<b>a</b>) Schematic diagram illustrating the modification process of Ce-RENPs@SiO<sub>2</sub>-RB/FA; (<b>b</b>) Ce-RENPs-RB/FA probes with dual-functional NIR-II in vivo imaging and ROS response and their corresponding UCL/DSL emissions; (<b>c</b>) UCL of the Ce-RENPs and the absorption of the RB; (<b>d</b>) hydrodynamic diameters and zeta potentials of Ce-RENPs-OA, Ce-RENPs@SiO<sub>2</sub>-NH<sub>2</sub>, Ce-RENPs@SiO<sub>2</sub>-RB, and Ce-RENPs@SiO<sub>2</sub>-RB/FA. Fluorogenic interactions between SOSG and <sup>1</sup>O<sub>2</sub>, generated by photoirradiation of Ce-RENPs@SiO<sub>2</sub>-RB; (<b>e</b>) fluorescence emission spectra of RB and SOSG before irradiation and a mixture of RB and SOSG before and at different time points after 980 nm irradiation; (<b>f</b>) dependence of the fluorescence intensity on 980 nm irradiation time.</p> "> Figure 8
<p>(<b>a</b>) Confocal fluorescence imaging of co-cultured HeLa cells with 50 μg/mL Ce-RENPs-RB/FA nanoprobes synthesized by the LBL/SA strategy and 50 μM SOSG under 980 nm excitation for 5 min and 10 min; (<b>b</b>) intensity ratio of confocal fluorescence between SOSG and RB; (<b>c</b>) NIR-II fluorescence imaging of subcutaneously injected mice treated with Ce-RENPs-SA (left circle) and Ce-RENPs-LBL (right circle) under 980 nm laser irradiation; (<b>d</b>) the NIR-II fluorescence imaging intensity values of Ce-RENPs-LBL/SA in mice.</p> ">
Abstract
:1. Introduction
2. Materials and Methods
2.1. Materials
2.2. Composition of RENPs
2.3. Method 1: One-Pot Successive LBL Strategy
2.3.1. Syntheses of Ce-RENPs Shell Precursors
2.3.2. Synthesis of Ce-RENPs Core
2.3.3. Synthesis of Ce-RENPs-LBL Core@Shell 1 with Different Thicknesses of Shell 1
2.3.4. Synthesis of Ce-RENPs-LBL Core@Shell 1@Shell 2
2.4. Method 2: Modified SA Growth Strategy
2.4.1. Synthesis of Ce-RENPs Core
2.4.2. Syntheses of Ce-RENPs Shell 1 Precursor and Shell 2 Precursor
2.4.3. Synthesis of Ce-RENPs-SA Core@Shell 1 with Different Thicknesses of Shell 1
2.4.4. Synthesis of Ce-RENPs-SA Core@Shell 1@Shell 2
2.5. Synthesis of Ce-RENPs@SiO2-NH2
2.6. Synthesis of Ce-RENPs@SiO2-RB/FA
2.7. Cell Culture
2.8. ROS Detection
2.9. In Vivo Imaging
2.10. Characterization
3. Results and Discussion
3.1. Synthesis Strategies and the Interface Characteristics
3.2. Interface Clarity and Energy Transfer
3.3. The Orthogonality of Luminescence and the Thickness of the Isolation Layer
3.4. ROS Generation and Detection of Ce-RENPs@SiO2-RB In Vitro and In Vivo
3.5. Enhanced NIR-II Imaging for SA Strategy
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
Abbreviations
RENPs | Rare Earth Nanoparticles |
LBL | Layer-by-Layer |
SA | Seed-Assisted |
NIR | Near Infrared |
PDT | Photodynamic Therapy |
ROS | Reactive Oxygen Species |
TEM | Transmission Electron Microscopy |
HAADF-STEM | High-angle annular dark-field scanning transmission electron microscopy |
EDXS | Energy dispersive X-ray spectroscopy |
XRD | X-ray diffraction |
UCL | Upconversion luminescence |
DSL | Down-shifting luminescence |
Tm-RENPs | Tm3+-doped RENPs |
Tm-RENPs-LBL | Tm-RENPs synthesized by LBL strategy |
Tm-RENPs-SA | Tm-RENPs synthesized by SA strategy |
Er-RENPs | Er3+-doped RENPs |
Er-RENPs-LBL | Er-RENPs synthesized by LBL strategy |
Er-RENPs-SA | Er-RENPs synthesized by SA strategy |
Ce-RENPs | Ce3+-doped RENPs |
Ce-RENPs-LBL | Ce-RENPs synthesized by LBL strategy |
Ce-RENPs-SA | Ce-RENPs synthesized by SA strategy |
NHS | N-hydroxy succinimide |
EDC | 1-ethyl-(3-dimethyllaminopropyl) carbodiimide hydrochloride |
HEPES | 2-[4-(2-hydroxyethyl)-1-piperazinyl] ethanesulfonic acid |
DMF | N,N-dimethylformamide |
APTES | 3-aminopropyl triethoxysilane |
RB | Rose Bengal |
FA | Folic acid |
SOSG | Singlet oxygen sensor green reagent |
CLSM | Confocal laser scanning microscope |
LED | Light-emitting diode |
Appendix A
Type of RENPs | Core Composition | Shell 1 Composition | Shell 2 Composition |
---|---|---|---|
Tm-RENPs | NaYF4: 0.5% Tm, 30% Yb | NaYF4: 10% Yb, 30% Nd | - |
Er-RENPs | NaYF4: 2% Er, 20% Yb | NaYF4: 5% Nd | - |
Ce-RENPs | NaYF4: 20% Ce, 2% Er, 20% Yb | NaYF4 | NaYF4: 5% Nd |
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Zhou, Z.; Liu, Y.; Guo, L.; Wang, T.; Yan, X.; Wei, S.; Qiu, D.; Chen, D.; Zhang, X.; Ju, H. Core–Shell Interface Engineering Strategies for Modulating Energy Transfer in Rare Earth-Doped Nanoparticles. Nanomaterials 2024, 14, 1326. https://doi.org/10.3390/nano14161326
Zhou Z, Liu Y, Guo L, Wang T, Yan X, Wei S, Qiu D, Chen D, Zhang X, Ju H. Core–Shell Interface Engineering Strategies for Modulating Energy Transfer in Rare Earth-Doped Nanoparticles. Nanomaterials. 2024; 14(16):1326. https://doi.org/10.3390/nano14161326
Chicago/Turabian StyleZhou, Zhaoxi, Yuan Liu, Lichao Guo, Tian Wang, Xinrong Yan, Shijiong Wei, Dehui Qiu, Desheng Chen, Xiaobo Zhang, and Huangxian Ju. 2024. "Core–Shell Interface Engineering Strategies for Modulating Energy Transfer in Rare Earth-Doped Nanoparticles" Nanomaterials 14, no. 16: 1326. https://doi.org/10.3390/nano14161326