Radioisotope post-labeling upconversion nanophosphors for in vivo quantitative tracking.

Lanthanide based upconversion nanophosphors (UCNPs) attracted increasing attention for potential applications in bioimaging, while its in vivo behaviors are not clear until now due to no available quantification imaging tools. Herein, we developed a unique rare-earth cation-exchange-based postlabelling method to introduce (153)Sm into the lattice of UCNPs, providing this (153)Sm-postlabeling UCNP having bifunction of radioactive property and upconversion luminescence under excitation at 980 nm laser. This (153)Sm-postlabelling method shows rapid treatment time of <1 min, high labeling yield of >99%, and without usage of organic solvents. More importantly, this (153)Sm-postlabelling method is also suitable for most of rare earth nanoparticles to track their in vivo behaviors. The dynamic quantification studies of the in vivo fate of the rare-earth nanoparticles were further investigated by radioactive detection method such as single-photon emission computed tomography (SPECT) and gamma counter. The imaging results revealed that UCNPs were mainly captured by the mononuclear phagocyte system (liver and spleen). The amount of nanoparticles in liver arrived at its peak quicker and was about 15 fold of that in spleen. And the nanoparticles will be slowly excreted with the bile. Therefore, the concept of postlabeling (153)Sm onto lanthanide-based UCNPs may serve as a facile strategy of fabricating multifunctional nanoprobes for upconversion luminescence (UCL) and SPECT dual-modality imaging.

[1]  Cunhai Dong,et al.  Cation exchange in lanthanide fluoride nanoparticles. , 2009, ACS nano.

[2]  Lehui Lu,et al.  A high-performance ytterbium-based nanoparticulate contrast agent for in vivo X-ray computed tomography imaging. , 2012, Angewandte Chemie.

[3]  Wei Feng,et al.  Blue-emissive upconversion nanoparticles for low-power-excited bioimaging in vivo. , 2012, Journal of the American Chemical Society.

[4]  Shuk Han Cheng,et al.  Polymer-coated NaYF₄:Yb³⁺, Er³⁺ upconversion nanoparticles for charge-dependent cellular imaging. , 2011, ACS nano.

[5]  Nora Khanarian,et al.  In vivo and scanning electron microscopy imaging of up-converting nanophosphors in Caenorhabditis elegans. , 2006, Nano letters.

[6]  Zhuang Liu,et al.  Near-infrared light induced in vivo photodynamic therapy of cancer based on upconversion nanoparticles. , 2011, Biomaterials.

[7]  Wei Feng,et al.  Cubic sub-20 nm NaLuF(4)-based upconversion nanophosphors for high-contrast bioimaging in different animal species. , 2012, Biomaterials.

[8]  Greg J. Stanisz,et al.  Size-Tunable, Ultrasmall NaGdF4 Nanoparticles: Insights into Their T1 MRI Contrast Enhancement , 2011 .

[9]  Jun Lin,et al.  Monodisperse core-shell structured up-conversion Yb(OH)CO₃@YbPO₄:Er³+ hollow spheres as drug carriers. , 2011, Biomaterials.

[10]  Renfu Li,et al.  Time-resolved FRET biosensor based on amine-functionalized lanthanide-doped NaYF4 nanocrystals. , 2011, Angewandte Chemie.

[11]  John E. Roberts,et al.  Lanthanum and Neodymium Salts of Trifluoroacetic Acid , 1961 .

[12]  Zhuang Liu,et al.  Upconversion nanophosphors for small-animal imaging. , 2012, Chemical Society reviews.

[13]  G. Stucky,et al.  Multiplexed Biological Detection: Fluorescence Upconversion Microbarcodes for Multiplexed Biological Detection: Nucleic Acid Encoding (Adv. Mater. 33/2011) , 2011 .

[14]  B. Tomanek,et al.  Cation Exchange: A Facile Method To Make NaYF4:Yb,Tm-NaGdF4 Core–Shell Nanoparticles with a Thin, Tunable, and Uniform Shell , 2012 .

[15]  C. Hawker,et al.  The Advantages of Nanoparticles for PET , 2009, Journal of Nuclear Medicine.

[16]  Xueyuan Chen,et al.  Upconversion nanoparticles in biological labeling, imaging, and therapy. , 2010, The Analyst.

[17]  Yanqing Hua,et al.  Multifunctional nanoprobes for upconversion fluorescence, MR and CT trimodal imaging. , 2012, Biomaterials.

[18]  Helmut Schäfer,et al.  Upconverting nanoparticles. , 2011, Angewandte Chemie.

[19]  Sanjiv S Gambhir,et al.  Cardiovascular molecular imaging. , 2007, Radiology.

[20]  Yongsheng Liu,et al.  A Strategy to Achieve Efficient Dual‐Mode Luminescence of Eu3+ in Lanthanides Doped Multifunctional NaGdF4 Nanocrystals , 2010, Advanced materials.

[21]  Yun Sun,et al.  Fluorine-18 labeled rare-earth nanoparticles for positron emission tomography (PET) imaging of sentinel lymph node. , 2011, Biomaterials.

[22]  A. Speghini,et al.  Colloidal Tm3+/Yb3+‐Doped LiYF4 Nanocrystals: Multiple Luminescence Spanning the UV to NIR Regions via Low‐Energy Excitation , 2009 .

[23]  Wei Feng,et al.  Sub-10 nm hexagonal lanthanide-doped NaLuF4 upconversion nanocrystals for sensitive bioimaging in vivo. , 2011, Journal of the American Chemical Society.

[24]  Shan Jiang,et al.  Multicolor Core/Shell‐Structured Upconversion Fluorescent Nanoparticles , 2008 .

[25]  Shiwei Wu,et al.  Non-blinking and photostable upconverted luminescence from single lanthanide-doped nanocrystals , 2009, Proceedings of the National Academy of Sciences.

[26]  Paras N. Prasad,et al.  (α-NaYbF4:Tm(3+))/CaF2 core/shell nanoparticles with efficient near-infrared to near-infrared upconversion for high-contrast deep tissue bioimaging. , 2012, ACS nano.

[27]  Mingdong Huang,et al.  Amine-functionalized lanthanide-doped KGdF4 nanocrystals as potential optical/magnetic multimodal bioprobes. , 2012, Journal of the American Chemical Society.

[28]  Yang Yang,et al.  Long-term in vivo biodistribution imaging and toxicity of polyacrylic acid-coated upconversion nanophosphors. , 2010, Biomaterials.

[29]  Fuyou Li,et al.  High contrast upconversion luminescence targeted imaging in vivo using peptide-labeled nanophosphors. , 2009, Analytical chemistry.

[30]  O. Wolfbeis,et al.  Upconverting luminescent nanoparticles for use in bioconjugation and bioimaging. , 2010, Current opinion in chemical biology.

[31]  I. Y. Chen,et al.  Cardiovascular molecular imaging: focus on clinical translation. , 2011, Circulation.

[32]  F. Auzel.  Upconversion and anti-Stokes processes with f and d ions in solids. , 2004, Chemical reviews.

[33]  Taeghwan Hyeon,et al.  Nonblinking and Nonbleaching Upconverting Nanoparticles as an Optical Imaging Nanoprobe and T1 Magnetic Resonance Imaging Contrast Agent , 2009 .

[34]  Fan Zhang,et al.  Fluorescence Upconversion Microbarcodes for Multiplexed Biological Detection: Nucleic Acid Encoding , 2011, Advanced materials.

[35]  Zhen Cheng,et al.  In vitro and in vivo uncaging and bioluminescence imaging by using photocaged upconversion nanoparticles. , 2012, Angewandte Chemie.

[36]  En Ma,et al.  Amine-functionalized lanthanide-doped zirconia nanoparticles: optical spectroscopy, time-resolved fluorescence resonance energy transfer biodetection, and targeted imaging. , 2012, Journal of the American Chemical Society.

[37]  Yong Zhang,et al.  Upconversion fluorescence imaging of cells and small animals using lanthanide doped nanocrystals. , 2008, Biomaterials.

[38]  Yuan Gao,et al.  Water-soluble NaYF4:Yb/Er upconversion nanophosphors: Synthesis, characteristics and application in bioimaging , 2010 .

[39]  Chun-Hua Yan,et al.  Bioimaging and toxicity assessments of near-infrared upconversion luminescent NaYF4:Yb,Tm nanocrystals. , 2011, Biomaterials.

[40]  Tymish Y. Ohulchanskyy,et al.  High contrast in vitro and in vivo photoluminescence bioimaging using near infrared to near infrared up-conversion in Tm3+ and Yb3+ doped fluoride nanophosphors. , 2008, Nano letters.

[41]  Qing Peng,et al.  Lanthanide-doped nanocrystals: synthesis, optical-magnetic properties, and applications. , 2011, Accounts of chemical research.

[42]  C. S. Lim,et al.  Simultaneous phase and size control of upconversion nanocrystals through lanthanide doping , 2010, Nature.

[43]  Yadong Yin,et al.  Cation Exchange Reactions in Ionic Nanocrystals , 2004, Science.

[44]  Jun Lin,et al.  Rare earth fluoride nano-/microcrystals: synthesis, surface modification and application , 2010 .

[45]  Kai Yang,et al.  In vivo pharmacokinetics, long-term biodistribution and toxicology study of functionalized upconversion nanoparticles in mice. , 2011, Nanomedicine.

[46]  Ya-Wen Zhang,et al.  High-quality sodium rare-earth fluoride nanocrystals: controlled synthesis and optical properties. , 2006, Journal of the American Chemical Society.

[47]  G. Chow,et al.  Synthesis of Hexagonal‐Phase NaYF4:Yb,Er and NaYF4:Yb,Tm Nanocrystals with Efficient Up‐Conversion Fluorescence , 2006 .

[48]  Yong Zhang,et al.  Biocompatibility of silica coated NaYF(4) upconversion fluorescent nanocrystals. , 2008, Biomaterials.