NDLI: Analysis of the isomer ratios of polymethylated-DOTA complexes and the implications on protein structural studies

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Analysis of the isomer ratios of polymethylated-DOTA complexes and the implications on protein structural studies

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Opina, Ana Christina L. Lee, Yong-sok Tjandra, Nico Vasalatiy, Olga Strickland, Madeleine Swenson, Rolf E. Andrew Byrd, R.
Description	Author Affiliation: Opina AC ( Imaging Probe Development Center, National Heart, Lung, and Blood Institute, National Institutes of Health, Rockville, MD 20850, USA. ana.opina@nih.gov.)
Abstract	A rigidified and symmetrical polymethylated 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA) ligand bearing four SSSS methyl groups in both the tetraaza ring and the acetate arms (SSSS-SSSS-M4DOTMA) was prepared. The isomer ratio of SSSS-SSSS-M4DOTMA complexed with a series of lanthanide ions was carefully investigated using RP-HPLC and NMR. A square antiprismatic (SAP) configuration was exclusively observed for the early lanthanides, while the twisted square antiprismatic (TSAP) geometry was preferred as the lanthanide ion size decreases. The late lanthanides preferentially adopted the TSAP geometry. One of the pendant arms was modified with a pyridyl disulfide group (SSSS-SSSS-M8SPy) for cysteine attachment and displayed a similar isomer trend as the parent compound, Ln-SSSS-SSSS-M4DOTMA. Covalent attachment to the ubiquitin S57C mutant showed resonances whose intensities are in agreement with the isomeric population observed by RP-HPLC. Furthermore, the NOE experiments combined with quantum chemical calculations have unequivocally demonstrated that the SAP of Pr-SSSS-SSSS-M4DOTMA and Pr-SSSS-SSSS-M8SPy, as well as the TSAP of Yb-SSSS-SSSS-M8SPy are more stable than their corresponding isomers.
ISSN	14779226
e-ISSN	13645447
Journal	Dalton Trans.
Issue Number	11
Volume Number	45
Language	English
Publisher	Royal Society of Chemistry
Publisher Date	2016-03-21
Publisher Place	Great Britain (UK)
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Inorganic Chemistry

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