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Title: 3,4,3-LI(1,2-HOPO): In Vitro Formation of Highly Stable Lanthanide Complexes Translates into Efficacious In Vivo Europium Decorporation

Abstract

The spermine-based hydroxypyridonate octadentate chelator 3,4,3-LI(1,2-HOPO) was investigated for its ability to act as an antennae that sensitizes the emission of Sm{sup III}, Eu{sup III}, and Tb{sup III} in the Visible range (Φ{sub tot} = 0.2 - 7%) and the emission of Pr{sup III}, Nd{sup III}, Sm{sup III}, and Yb{sup III} in the Near Infra-Red range, with decay times varying from 1.78 μs to 805 μs at room temperature. The particular luminescence spectroscopic properties of these lanthanide complexes formed with 3,4,3-LI(1,2-HOPO) were used to characterize their respective solution thermodynamic stabilities as well as those of the corresponding La{sup III}, Gd{sup III}, Dy{sup III}, Ho{sup III}, Er{sup III}, Tm{sup III}, and Lu{sup III} complexes. The remarkably high affinity of 3,4,3-LI(1,2-HOPO) for lanthanide metal ions and the resulting high complex stabilities (pM values ranging from 17.2 for La{sup III} to 23.1 for Yb{sup III}) constitute a necessary but not sufficient criteria to consider this octadentate ligand an optimal candidate for in vivo metal decorporation. The in vivo lanthanide complex stability and decorporation capacity of the ligand were assessed, using the radioactive isotope {sup 152}Eu as a tracer in a rodent model, which provided a direct comparison with the in vitro thermodynamic resultsmore » and demonstrated the great potential of 3,4,3-LI(1,2-HOPO) as a therapeutic metal chelating agent.« less

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
Chemical Sciences Division
OSTI Identifier:
1051843
Report Number(s):
LBNL-5195E
Journal ID: ISSN 1477--9226
DOE Contract Number:  
DE-AC02-05CH11231
Resource Type:
Journal Article
Journal Name:
Dalton Transactions
Additional Journal Information:
Journal Volume: 40; Journal Issue: 33; Journal ID: ISSN 1477--9226
Country of Publication:
United States
Language:
English
Subject:
60 APPLIED LIFE SCIENCES; 59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sturzbecher-Hoehne, Manuel, Ng Pak Leung, Clara, Daleo, Anthony, Kullgren, Birgitta, Prigent, Anne-Laure, Shuh, David K., Raymond, Kenneth N., and Abergel, Rebecca J. 3,4,3-LI(1,2-HOPO): In Vitro Formation of Highly Stable Lanthanide Complexes Translates into Efficacious In Vivo Europium Decorporation. United States: N. p., 2011. Web. doi:10.1039/c1dt10840a.
Sturzbecher-Hoehne, Manuel, Ng Pak Leung, Clara, Daleo, Anthony, Kullgren, Birgitta, Prigent, Anne-Laure, Shuh, David K., Raymond, Kenneth N., & Abergel, Rebecca J. 3,4,3-LI(1,2-HOPO): In Vitro Formation of Highly Stable Lanthanide Complexes Translates into Efficacious In Vivo Europium Decorporation. United States. doi:10.1039/c1dt10840a.
Sturzbecher-Hoehne, Manuel, Ng Pak Leung, Clara, Daleo, Anthony, Kullgren, Birgitta, Prigent, Anne-Laure, Shuh, David K., Raymond, Kenneth N., and Abergel, Rebecca J. Wed . "3,4,3-LI(1,2-HOPO): In Vitro Formation of Highly Stable Lanthanide Complexes Translates into Efficacious In Vivo Europium Decorporation". United States. doi:10.1039/c1dt10840a. https://www.osti.gov/servlets/purl/1051843.
@article{osti_1051843,
title = {3,4,3-LI(1,2-HOPO): In Vitro Formation of Highly Stable Lanthanide Complexes Translates into Efficacious In Vivo Europium Decorporation},
author = {Sturzbecher-Hoehne, Manuel and Ng Pak Leung, Clara and Daleo, Anthony and Kullgren, Birgitta and Prigent, Anne-Laure and Shuh, David K. and Raymond, Kenneth N. and Abergel, Rebecca J.},
abstractNote = {The spermine-based hydroxypyridonate octadentate chelator 3,4,3-LI(1,2-HOPO) was investigated for its ability to act as an antennae that sensitizes the emission of Sm{sup III}, Eu{sup III}, and Tb{sup III} in the Visible range (Φ{sub tot} = 0.2 - 7%) and the emission of Pr{sup III}, Nd{sup III}, Sm{sup III}, and Yb{sup III} in the Near Infra-Red range, with decay times varying from 1.78 μs to 805 μs at room temperature. The particular luminescence spectroscopic properties of these lanthanide complexes formed with 3,4,3-LI(1,2-HOPO) were used to characterize their respective solution thermodynamic stabilities as well as those of the corresponding La{sup III}, Gd{sup III}, Dy{sup III}, Ho{sup III}, Er{sup III}, Tm{sup III}, and Lu{sup III} complexes. The remarkably high affinity of 3,4,3-LI(1,2-HOPO) for lanthanide metal ions and the resulting high complex stabilities (pM values ranging from 17.2 for La{sup III} to 23.1 for Yb{sup III}) constitute a necessary but not sufficient criteria to consider this octadentate ligand an optimal candidate for in vivo metal decorporation. The in vivo lanthanide complex stability and decorporation capacity of the ligand were assessed, using the radioactive isotope {sup 152}Eu as a tracer in a rodent model, which provided a direct comparison with the in vitro thermodynamic results and demonstrated the great potential of 3,4,3-LI(1,2-HOPO) as a therapeutic metal chelating agent.},
doi = {10.1039/c1dt10840a},
journal = {Dalton Transactions},
issn = {1477--9226},
number = 33,
volume = 40,
place = {United States},
year = {2011},
month = {7}
}