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Title: Synthesis and characterization of intrinsically radiolabeled lanthanide phosphate nanoparticles toward biomedical and environmental applications

Abstract

Lanthanide phosphate nanomaterials are appealing as multifunctional platforms for biomedical applications because of their low toxicity, radiation resistance, and unique luminescence and magnetic properties. Lanthanide phosphate nanoparticles (NPs) radiolabeled with 156Eu were synthesized by an aqueous route using sodium tripolyphosphate as a phosphate source and complexing agent. GdPO4 was used as a host matrix, while synthetic concentrations of Ce3+/Tb3+ and Eu3+ were varied between 5–40% and 10–30%, respectively, and yielded spherical NPs with hexagonal crystal system and particle size < 5 nm. Luminescence emission and magnetic susceptibility were influenced by lanthanide concentrations where characteristic 5D0-7FJ and 5D4-7FJ transitions were observed for Eu3+- and Tb3+-doped NPs, respectively. Chemical yield of > 90% was achieved for GdPO4 and Gd0.6Ce0.3Tb0.1PO4 NPs intrinsically radiolabeled with 156Eu. Lastly, in vitro retention of 156Eu within LnPO4 NPs was > 97% over 3 weeks. Intrinsically radiolabeled LnPO4 NPs have the potential to combine the luminescence and magnetic properties of Ln3+ ions with lanthanide radioisotopes for biomedical and environmental applications.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [2];  [1]
  1. Virginia Commonwealth Univ., Richmond, VA (United States). Dept. of Mechanical and Nuclear Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Nuclear Security and Isotope Technology Division
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1471921
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Nanoparticle Research
Additional Journal Information:
Journal Volume: 20; Journal Issue: 9; Journal ID: ISSN 1388-0764
Publisher:
Tsinghua University Press
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; Multifunctional nanomaterials; lanthanide phosphate; luminescence; magnetic susceptibility; intrinsically radiolabeled nanoparticles; europium-156

Citation Formats

Toro Gonzalez, Miguel T., Clifford, Dustin M., Copping, Roy, Mirzadeh, Saed, and Rojas, Jessika V. Synthesis and characterization of intrinsically radiolabeled lanthanide phosphate nanoparticles toward biomedical and environmental applications. United States: N. p., 2018. Web. doi:10.1007/s11051-018-4338-8.
Toro Gonzalez, Miguel T., Clifford, Dustin M., Copping, Roy, Mirzadeh, Saed, & Rojas, Jessika V. Synthesis and characterization of intrinsically radiolabeled lanthanide phosphate nanoparticles toward biomedical and environmental applications. United States. https://doi.org/10.1007/s11051-018-4338-8
Toro Gonzalez, Miguel T., Clifford, Dustin M., Copping, Roy, Mirzadeh, Saed, and Rojas, Jessika V. Thu . "Synthesis and characterization of intrinsically radiolabeled lanthanide phosphate nanoparticles toward biomedical and environmental applications". United States. https://doi.org/10.1007/s11051-018-4338-8. https://www.osti.gov/servlets/purl/1471921.
@article{osti_1471921,
title = {Synthesis and characterization of intrinsically radiolabeled lanthanide phosphate nanoparticles toward biomedical and environmental applications},
author = {Toro Gonzalez, Miguel T. and Clifford, Dustin M. and Copping, Roy and Mirzadeh, Saed and Rojas, Jessika V.},
abstractNote = {Lanthanide phosphate nanomaterials are appealing as multifunctional platforms for biomedical applications because of their low toxicity, radiation resistance, and unique luminescence and magnetic properties. Lanthanide phosphate nanoparticles (NPs) radiolabeled with 156Eu were synthesized by an aqueous route using sodium tripolyphosphate as a phosphate source and complexing agent. GdPO4 was used as a host matrix, while synthetic concentrations of Ce3+/Tb3+ and Eu3+ were varied between 5–40% and 10–30%, respectively, and yielded spherical NPs with hexagonal crystal system and particle size < 5 nm. Luminescence emission and magnetic susceptibility were influenced by lanthanide concentrations where characteristic 5D0-7FJ and 5D4-7FJ transitions were observed for Eu3+- and Tb3+-doped NPs, respectively. Chemical yield of > 90% was achieved for GdPO4 and Gd0.6Ce0.3Tb0.1PO4 NPs intrinsically radiolabeled with 156Eu. Lastly, in vitro retention of 156Eu within LnPO4 NPs was > 97% over 3 weeks. Intrinsically radiolabeled LnPO4 NPs have the potential to combine the luminescence and magnetic properties of Ln3+ ions with lanthanide radioisotopes for biomedical and environmental applications.},
doi = {10.1007/s11051-018-4338-8},
journal = {Journal of Nanoparticle Research},
number = 9,
volume = 20,
place = {United States},
year = {Thu Sep 06 00:00:00 EDT 2018},
month = {Thu Sep 06 00:00:00 EDT 2018}
}

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Figures / Tables:

Fig. 1 Fig. 1: Diffraction patterns of (a) GdPO4 (blue), (b) Gd0.9Eu0.1PO4 (orange), (c) Gd0.7Eu0.3PO4 (yellow), (d) Gd0.95Ce0.0375Tb0.0125PO4 (purple), (e) Gd0.6Ce0.3Tb0.1PO4 (green), and (f) GdPO4·nH2O (black).

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Works referenced in this record:

Probing the effect of radiation damage on the structure of rare-earth phosphates
journal, December 2015


Aqueous routes to lanthanide-doped oxide nanophosphors
journal, January 2006

  • Buissette, Valérie; Giaume, Domitille; Gacoin, Thierry
  • J. Mater. Chem., Vol. 16, Issue 6
  • DOI: 10.1039/b508656f

Synthesis and Fluorescence Properties of Europium-Lanthanum-Calcium Orthophosphates and Condensed Phosphates
journal, January 2012

  • Onoda, Hiroaki; Funamoto, Takehiro
  • Advances in Materials Physics and Chemistry, Vol. 02, Issue 04
  • DOI: 10.4236/ampc.2012.24031

Facile preparation and bifunctional imaging of Eu-doped GdPO 4 nanorods with MRI and cellular luminescence
journal, January 2015

  • Du, Qijun; Huang, Zhongbing; Wu, Zhi
  • Dalton Transactions, Vol. 44, Issue 9
  • DOI: 10.1039/c4dt03444a

Lanthanide and Actinide Chemistry
book, January 2006


Gold Coated Lanthanide Phosphate Nanoparticles for Targeted Alpha Generator Radiotherapy
journal, January 2013


Application of radioisotopes in the field of nuclear medicine: I. Lanthanide series elements
journal, November 1999

  • Nayak, D.; Lahiri, S.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 242, Issue 2
  • DOI: 10.1007/BF02345573

Current and Potential Therapeutic Uses of Lanthanide Radioisotopes
journal, December 2000

  • Cutler, Cathy S.; Smith, C. Jeffrey; Ehrhardt, Gary J.
  • Cancer Biotherapy and Radiopharmaceuticals, Vol. 15, Issue 6
  • DOI: 10.1089/cbr.2000.15.531

A facile route for preparing rhabdophane rare earth phosphate nanorods
journal, January 2006

  • Wang, Xiaojuan; Gao, Mingyuan
  • Journal of Materials Chemistry, Vol. 16, Issue 14
  • DOI: 10.1039/b517179b

Diamagnetic Corrections and Pascal's Constants
journal, April 2008

  • Bain, Gordon A.; Berry, John F.
  • Journal of Chemical Education, Vol. 85, Issue 4
  • DOI: 10.1021/ed085p532

Nanomaterials: Applications in Cancer Imaging and Therapy
journal, February 2011

  • Barreto, José A.; O’Malley, William; Kubeil, Manja
  • Advanced Materials, Vol. 23, Issue 12
  • DOI: 10.1002/adma.201100140

Tripolyphosphate as Precursor for REPO4:Eu3+ (RE = Y, La, Gd) by a Polymeric Method
journal, November 2007


Multi-isotope SPECT imaging of the 225 Ac decay chain: feasibility studies
journal, May 2017

  • Robertson, A. K. H.; Ramogida, C. F.; Rodríguez-Rodríguez, C.
  • Physics in Medicine and Biology, Vol. 62, Issue 11
  • DOI: 10.1088/1361-6560/aa6a99

Hydrothermal synthesis and luminescent properties of LnPO4:Tb,Bi (Ln=La,Gd) phosphors under UV/VUV excitation
journal, October 2007


Luminescent-plasmonic effects in GdPO 4 :Eu 3+ nanorods covered with silver nanoparticles
journal, August 2017


Colloidal Synthesis of Luminescent Rhabdophane LaPO 4 :Ln 3+ · x H 2 O (Ln = Ce, Tb, Eu; x ≈ 0.7) Nanocrystals
journal, September 2004

  • Buissette, Valérie; Moreau, Mélanie; Gacoin, Thierry
  • Chemistry of Materials, Vol. 16, Issue 19
  • DOI: 10.1021/cm049323a

Gd2O3 nanoparticles stabilized by hydrothermally modified dextrose for positive contrast magnetic resonance imaging
journal, April 2016

  • Babić-Stojić, Branka; Jokanović, Vukoman; Milivojević, Dušan
  • Journal of Magnetism and Magnetic Materials, Vol. 403
  • DOI: 10.1016/j.jmmm.2015.11.075

Paramagnetic nanoparticles as potential MRI contrast agents: characterization, NMR relaxation, simulations and theory
journal, July 2012

  • Vuong, Quoc Lam; Van Doorslaer, Sabine; Bridot, Jean-Luc
  • Magnetic Resonance Materials in Physics, Biology and Medicine, Vol. 25, Issue 6
  • DOI: 10.1007/s10334-012-0326-7

Fabrication and characterization of the photoluminescent properties of Tb3+ doped one-dimensional GdPO4 nanorods
journal, September 2007


LnPO4: RE3+ (La = La, Gd; RE = Eu, Tb) nanocrystals: solvo-thermal synthesis, microstructure and photoluminescence
journal, October 2009


Probing of inversion symmetry site in Eu3+-doped GdPO4 by luminescence study: Concentration and annealing effect
journal, January 2010


Atomistic modeling and experimental studies of radiation damage in monazite-type LaPO 4 ceramics
journal, February 2017

  • Ji, Yaqi; Kowalski, Piotr M.; Neumeier, Stefan
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 393
  • DOI: 10.1016/j.nimb.2016.09.031

Radiation resistance of LaPO4 (monazite structure) and YbPO4 (zircon structure) from data of computer simulation
journal, September 2013

  • Grechanovsky, A. E.; Eremin, N. N.; Urusov, V. S.
  • Physics of the Solid State, Vol. 55, Issue 9
  • DOI: 10.1134/S1063783413090138

Synthesis and targeting of gold-coated 177 Lu-containing lanthanide phosphate nanoparticles—A potential theranostic agent for pulmonary metastatic disease
journal, March 2018

  • Sobol, Nicholas; Sutherlin, Logan; Cedrowska, Edyta
  • APL Bioengineering, Vol. 2, Issue 1
  • DOI: 10.1063/1.5018165

Dextran Coated Gadolinium Phosphate Nanoparticles for Magnetic Resonance Tumor Imaging
journal, January 2009

  • Hifumi, Hiroki; Yamaoka, Seiichi; Tanimoto, Akihiro
  • Journal of Materials Chemistry, Vol. 19, Issue 35
  • DOI: 10.1039/b902134e

Multifunctional Rare-Earth Vanadate Nanoparticles: Luminescent Labels, Oxidant Sensors, and MRI Contrast Agents
journal, October 2014

  • Abdesselem, Mouna; Schoeffel, Markus; Maurin, Isabelle
  • ACS Nano, Vol. 8, Issue 11
  • DOI: 10.1021/nn504170x

Liquid-Phase Synthesis of Colloids and Redispersible Powders of Strongly Luminescing LaPO4:Ce,Tb Nanocrystals
journal, January 2001


LaPO 4 Nanoparticles Doped with Actinium-225 that Partially Sequester Daughter Radionuclides
journal, April 2011

  • Woodward, Jonathan; Kennel, Stephen J.; Stuckey, Alan
  • Bioconjugate Chemistry, Vol. 22, Issue 4
  • DOI: 10.1021/bc100574f

LnPO 4 Nanoparticles Doped with Ac-225 and Sequestered Daughters for Targeted Alpha Therapy
journal, February 2014

  • McLaughlin, Mark F.; Robertson, David; Pevsner, Paul H.
  • Cancer Biotherapy and Radiopharmaceuticals, Vol. 29, Issue 1
  • DOI: 10.1089/cbr.2013.1546

Lanthanide-doped GdVO4 upconversion nanophosphors with tunable emissions and their applications for biomedical imaging
journal, January 2012

  • Yin, Wenyan; Zhou, Liangjun; Gu, Zhanjun
  • Journal of Materials Chemistry, Vol. 22, Issue 14
  • DOI: 10.1039/c2jm16152d

Luminescent Core/Shell Nanoparticles with a Rhabdophane LnPO4-xH2O Structure: Stabilization of Ce3+-Doped Compositions
journal, February 2006

  • Buissette, V.; Moreau, M.; Gacoin, T.
  • Advanced Functional Materials, Vol. 16, Issue 3
  • DOI: 10.1002/adfm.200500285

Multifunctionality of GdPO4:Yb3+,Tb3+ nanocrystals – luminescence and magnetic behaviour
journal, January 2012

  • Grzyb, Tomasz; Gruszeczka, Aleksandra; Wiglusz, Rafal J.
  • Journal of Materials Chemistry, Vol. 22, Issue 43
  • DOI: 10.1039/c2jm34863b

Gadolinium-based contrast agent toxicity: a review of known and proposed mechanisms
journal, April 2016


Controlled synthesis and characterization of LaPO4, LaPO4:Ce3+ and LaPO4:Ce3+, Tb3+ by EDTA assisted hydrothermal method
journal, September 2010


Hydrothermal synthesis and photoluminescence of the monophosphate LaPO4:Eu(5%)
journal, November 2008


Lanthanides: Applications in Cancer Diagnosis and Therapy: Miniperspective
journal, February 2016


Solvent interface effect on the size and crystalline nature of the GdPO4:Eu3+ nanorods
journal, October 2015


The Scherrer equation versus the 'Debye-Scherrer equation'
journal, August 2011


Morphology and Crsytallization Control of Multifunctional GdPO<sub>4</sub>:Eu Nanostructures by Hydrothermal Preparation
journal, December 2014


Rare earth based nanostructured materials: synthesis, functionalization, properties and bioimaging and biosensing applications
journal, June 2017

  • Escudero, Alberto; Becerro, Ana I.; Carrillo-Carrión, Carolina
  • Nanophotonics, Vol. 6, Issue 5
  • DOI: 10.1515/nanoph-2017-0007

Lanthanide ion-doped GdPO4 nanorods with dual-modal bio-optical and magnetic resonance imaging properties
journal, January 2012

  • Ren, Wenlu; Tian, Gan; Zhou, Liangjun
  • Nanoscale, Vol. 4, Issue 12
  • DOI: 10.1039/c2nr30683b

Solvothermal synthesis and luminescent properties of monodisperse LaPO4:Ln (Ln=Eu3+, Ce3+, Tb3+) particles
journal, May 2009


Sonochemical synthesis and photoluminescence properties of rare-earth phosphate core/shell nanorods
journal, April 2010


Biological Applications of Rare-Earth Based Nanoparticles
journal, October 2011

  • Bouzigues, Cedric; Gacoin, Thierry; Alexandrou, Antigoni
  • ACS Nano, Vol. 5, Issue 11
  • DOI: 10.1021/nn202378b

DNA Surface Modified Gadolinium Phosphate Nanoparticles as MRI Contrast Agents
journal, April 2012

  • Dumont, Matthieu F.; Baligand, Celine; Li, Yichen
  • Bioconjugate Chemistry, Vol. 23, Issue 5
  • DOI: 10.1021/bc200553h

Synthesis and Properties of Multifunctional Tetragonal Eu:GdPO 4 Nanocubes for Optical and Magnetic Resonance Imaging Applications
journal, December 2012

  • Rodriguez-Liviano, Sonia; Becerro, Ana I.; Alcántara, David
  • Inorganic Chemistry, Vol. 52, Issue 2
  • DOI: 10.1021/ic3016996

Hydrothermal Synthesis, Microstructure and Photoluminescence of Eu3+-Doped Mixed Rare Earth Nano-Orthophosphates
journal, August 2010


Gadolinium-based contrast agents: A comprehensive risk assessment: Gadolinium Risk Assessment
journal, January 2017

  • Fraum, Tyler J.; Ludwig, Daniel R.; Bashir, Mustafa R.
  • Journal of Magnetic Resonance Imaging, Vol. 46, Issue 2
  • DOI: 10.1002/jmri.25625

Size-Dependent MRI Relaxivity and Dual Imaging with Eu 0.2 Gd 0.8 PO 4 ·H 2 O Nanoparticles
journal, May 2014

  • Li, Yichen; Chen, Tao; Tan, Weihong
  • Langmuir, Vol. 30, Issue 20
  • DOI: 10.1021/la500602x

Gold-coated lanthanide phosphate nanoparticles for an 225Ac in vivo alpha generator
journal, September 2013


A Structural Investigation of Hydrous and Anhydrous Rare-Earth Phosphates
journal, September 2016


Heat-treatment-induced luminescence degradation in Tb3+-doped CePO4 nanorods
journal, April 2010


Selective synthesis and luminescence property of monazite- and hexagonal-type LaPO4: Eu nanocrystals
journal, January 2009

  • Lai, Hua; Bao, Amurisana; Yang, Yuming
  • CrystEngComm, Vol. 11, Issue 6
  • DOI: 10.1039/b818877g

Synthesis and characterization of lanthanum phosphate nanoparticles as carriers for 223Ra and 225Ra for targeted alpha therapy
journal, July 2015


Luminescence, lifetime, and quantum yield studies of redispersible Eu3+-doped GdPO4 crystalline nanoneedles: Core-shell and concentration effects
journal, February 2010

  • Yaiphaba, N.; Ningthoujam, R. S.; Singh, N. Shanta
  • Journal of Applied Physics, Vol. 107, Issue 3
  • DOI: 10.1063/1.3294964

Gadolinium-Based Contrast Agent Accumulation and Toxicity: An Update
journal, December 2015

  • Ramalho, J.; Semelka, R. C.; Ramalho, M.
  • American Journal of Neuroradiology, Vol. 37, Issue 7
  • DOI: 10.3174/ajnr.A4615

Core/shell-type nanorods of Tb3+-doped LaPO4, modified with amine groups, revealing reduced cytotoxicity
journal, October 2013

  • Runowski, Marcin; Dąbrowska, Krystyna; Grzyb, Tomasz
  • Journal of Nanoparticle Research, Vol. 15, Issue 11
  • DOI: 10.1007/s11051-013-2068-5

Lanthanide Nanoparticles: From Design toward Bioimaging and Therapy
journal, April 2015


Synthesis and Luminescent Properties of REVO 4 –REPO 4 (RE = Y, Eu, Gd, Er, Tm, or Yb) Heteronanostructures: A Promising Class of Phosphors for Excitation from NIR to VUV
journal, October 2015

  • de Sousa Filho, Paulo C.; Gacoin, Thierry; Boilot, Jean-Pierre
  • The Journal of Physical Chemistry C, Vol. 119, Issue 42
  • DOI: 10.1021/acs.jpcc.5b08249

Inter-atomic potentials for radiation damage studies in CePO 4 monazite
journal, February 2017

  • Jolley, Kenny; Asuvathraman, Rajaram; Smith, Roger
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 393
  • DOI: 10.1016/j.nimb.2016.10.016

Intrinsically radiolabeled multifunctional cerium oxide nanoparticles for in vivo studies
journal, January 2013

  • Yang, Likun; Sundaresan, Gobalakrishnan; Sun, Minghao
  • Journal of Materials Chemistry B, Vol. 1, Issue 10
  • DOI: 10.1039/c2tb00404f

Systematic Synthesis of Lanthanide Phosphate Nanocrystals
journal, September 2007

  • Huo, Ziyang; Chen, Chen; Chu, Deren
  • Chemistry - A European Journal, Vol. 13, Issue 27
  • DOI: 10.1002/chem.200601727

New insights into phosphate based materials for the immobilisation of actinides
journal, January 2017

  • Neumeier, Stefan; Arinicheva, Yulia; Ji, Yaqi
  • Radiochimica Acta, Vol. 105, Issue 11
  • DOI: 10.1515/ract-2017-2819

Engineering lanthanide-based materials for nanomedicine
journal, September 2014


Paramagnetic nanoparticle T1 and T2 MRI contrast agents
journal, January 2012

  • Xu, Wenlong; Kattel, Krishna; Park, Ja Young
  • Physical Chemistry Chemical Physics, Vol. 14, Issue 37
  • DOI: 10.1039/c2cp41357d

Morphology controllable and highly luminescent monoclinic LaPO4:Eu3+ microspheres
journal, January 2014


(Gd,Yb,Tb)PO4 up-conversion nanocrystals for bimodal luminescence–MR imaging
journal, January 2012

  • Debasu, Mengistie L.; Ananias, Duarte; Pinho, Sonia L. C.
  • Nanoscale, Vol. 4, Issue 16
  • DOI: 10.1039/c2nr31226c

Nanoparticle-based theranostic agents
journal, August 2010


Are Rare-Earth Nanoparticles Suitable for In Vivo Applications?
journal, March 2014


Colloidal Synthesis of Luminescent Rhabdophane LaPO4:Ln3+×xH2O (Ln: Ce, Tb, Eu; x ≈ 0.7) Nanocrystals.
journal, December 2004

  • Buissette, Valerie; Moreau, Melanie; Gacoin, Thierry
  • ChemInform, Vol. 35, Issue 49
  • DOI: 10.1002/chin.200449009

Generation of highly amenable cellulose-Iβ via selective delignification of rice straw using a reusable cyclic ether-assisted deep eutectic solvent system
journal, January 2021

  • Thulluri, Chiranjeevi; Balasubramaniam, Ravi; Velankar, Harshad Ravindra
  • Scientific Reports, Vol. 11, Issue 1
  • DOI: 10.1038/s41598-020-80719-x

Works referencing / citing this record:

Gadolinium vanadate nanocrystals as carriers of α-emitters ( 225 Ac, 227 Th) and contrast agents
journal, June 2019

  • Toro-González, Miguel; Dame, Ashley N.; Mirzadeh, Saed
  • Journal of Applied Physics, Vol. 125, Issue 21
  • DOI: 10.1063/1.5096880

Prediction of new iodine-containing apatites using machine learning and density functional theory
journal, August 2019

  • Hartnett, Timothy Q.; Ayyasamy, Mukil V.; Balachandran, Prasanna V.
  • MRS Communications, Vol. 9, Issue 3
  • DOI: 10.1557/mrc.2019.103