The structure and dynamics of the lanthanide(III) complexes
of DTPA-BGLUCA3- (DTPA-bis(glucamide)),
DTPA-BENGALAA3-
(DTPA-bis(ethylenegalactamine−amide)),
DTPA-BEA3- (DTPA-bis(ethanolamide)), and
DTPA-BPDA3- (DTPA-bis(propanediolamide)) in
water have been investigated. These complexes are of relevance
as
potential MRI contrast agents. 13C relaxation times of
the Nd(III) complexes show octadentate binding of the
organic ligand via the three amines, the three carboxylates, and the
two amide oxygens. 17O NMR measurements
indicate that the coordination sphere is completed by one water ligand.
Eight diastereomeric pairs of isomers are
observed for the DTPA-bis(sugaramides). Data sets obtained
from variable-temperature and -pressure 17O
NMR
at 9.4 T and variable-temperature 1H nuclear magnetic
relaxation dispersion (NMRD) on the Gd(III) complexes
were fitted simultaneously to give insight into the parameters
governing the water 1H relaxivity. The
water
exchange rates, k
ex
298, on
[Gd(DTPA-BPDA)(H2O)],
[Gd(DTPA-BGLUCA)(H2O)] and
[Gd(DTPA-BENGALAA)(H2O)] are 3.6 ± 0.3, 3.8 ± 0.2, and 2.2 ± 0.1 ×
105 s-1, and the activation
volumes are +6.7, +6.8, and +5.6
cm3 mol-1 (±0.2 cm3
mol-1), respectively, indicating a strongly
dissociatively activated mechanism. The sugar
moieties have no significant influence on the coordination of the
Gd(III) ion and on the parameters governing the
relaxivity, apart from the expected increase in the rotational
correlation time. The relaxivity under the usual
MRI conditions is limited by the water exchange rate and the electronic
relaxation. The data obtained are used
to explain the relaxivity of conjugates of polysaccharides and
Gd(DTPA).
The Gd3+ complexes of three new phosphorus containing tetraaza macrocycles (1,4,7,10-tetraazacyclododecane-1,4,7,10-tetrakis (methylene ethylphosphonic acid), H4DOTEP; 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetrakis (methylene phosphonic acid monoethylester), H4DOTPME; and the corresponding n-butyl ester, H4DOTPMB) were prepared and examined for possible use as MRI contrast agents. Although thermodynamically and kinetically less stable than Gd(DOTA)- in saline and HSA solution, the stability of these new macrocyclic complexes appears to be sufficiently high for in vivo applications. NMRD relaxivity profiles of the three complexes indicate that the number of inner sphere water molecules for these chelates is < or = 1 and that the more hydrophobic chelate, Gd(DOTPMB), binds to human serum albumin (HSA). Biodistribution studies of the radioactive 153Sm or 159Gd chelates in rats, gamma imaging of the 153Sm chelates in rats, and proton MRI studies of the nonradioactive Gd3+ chelates in rabbits all indicate that the DOTPMB complexes accumulate preferentially in the liver, spleen, and small intestines while the more hydrophilic DOTEP and DOTPME complexes appear to display renal clearances similar to other low molecular weight contrast agents.
Low-field (0.02--4 MHz) proton nuclear magnetic resonance (NMR) longitudinal relaxometry was applied to ultrahighly diluted aqueous solutions in order to detect physical modifications induced in the solvent by the dilution process. A mixture of silica-lactose (1.67.10 -5 M silica, 2.92-10 -2 M lactose) was initially solubilized in water or in saline, then submitted to eighteen iterative centesimal dilutions in water or in saline under vigorous vortex agitation and rigorously controlled atmospheric conditions, and compared to similarly treated pure water and saline as controls. Several independent series of samples were measured according to a blind protocol (total of 140 code-labelled samples). A slight frequency dispersion (about 4%) was found within the 0.02-4 MHz range, centered around 0.55 MHz, and ascribed to combined effects of silica and trace paramagnetic contaminants, both concentrated and in a reduced motion at the borosilicate wall tube interface. The iterative dilutionagitation process in pure water and saline induced no significant effect on relaxivity. Slightly increased relaxivity compared to solvent was found in the initial silica-lactose dilution (especially in saline, about 4%), which vanished unexpectedly slowly upon dilution, as adjusted to an arbitrary log-linear model. Statistical analysis was applied to succeed in discriminating solutions from their solvents beyond the 10 -~z level of dilution. No clear explanation emerged, but post-experiment chemical analysis revealed high amounts (6 ppm) of released silica from the glass mate¡ used, with excess in silicalactose samples, and lower amounts of trace paramagnetic contaminants in highly diluted silica-lactose samples, which could provide a clue.
The characterization of the hepatobiliary contrast agent Gd-EOB-DTPA (gadolinium 3, 6, 9-triaza-3, 6, 9-tris(carboxymethyl)-4-(4-ethoxybenzyl)-undecandicarboxylic acid) in various media (water solution, protein containing solution, phosphorylated metabolites solution, and excised and perfused liver) was performed using different NMR approaches: water 1H nuclear magnetic relaxation dispersion profiles, 2H NMR longitudinal and transverse relaxation rates of labeled complex, water 17O transverse relaxation rates and chemical shifts, 31P relaxation rates and peak area of phosphorylated metabolites. The higher proton relaxivity of Gd-EOB-DTPA in water compared with Gd-DTPA is related to a shorter distance (r) between the water proton and the gadolinium ion and to a longer rotational correlation time (tauR) of the hydrated complex. Although the thermodynamic stability of Gd-EOB-DTPA is identical to the one of Gd-DTPA, its kinetic stability in solutions containing phosphorylated metabolites (ATP, phosphocreatine, and inorganic phosphate) as measured by 31P relaxation rates analysis is higher than for the parent compound. Gd-EOB-DTPA binds noncovalently to serum proteins. Its interaction with human serum albumin is characterized by a dissociation constant of 1-4.1 mM as calculated from proton and deuterium relaxation rates and equilibrium dialysis. This noncovalent interaction involves the subdomain IIA of human serum albumin. 31P spectroscopy of the excised and perfused rat livers was used to monitor the uptake of Gd-EOB-DTPA by the hepatocytes where it enhances the nuclear relaxation of the intracellular metabolites without impairing the adenosine triphosphate metabolism of the cells.
OBJECTIVES:The present study aimed to assess the influence of dental occlusion on body posture and the competitive performance of young elite rowers.METHOD:Dental occlusion disturbance devices were used to simulate dental malocclusions. We assessed the influence of malocclusion on the body balance, paravertebral muscle contraction symmetry, and muscular power of young elite rowers. A nonparametric permutation test for repeated measures ANOVA, a Cochran's Q test for paired data and a paired Student's t-test were used in order to statistically evaluate the influence of artificial occlusal disturbance on each factor. A force platform and a Dyno Concept 2 machine were used as measuring instruments.RESULTS:A total of 7 members of the “Pôle France Aviron” (age range of 15-17 years) were enrolled in the study. None of the body balance parameters was significantly influenced by the artificial occlusal disturbance. The interposition of an occlusal silicone splint significantly increased the proportion of athletes presenting asymmetric muscular contractions from 14.3% to 85.7% (p=0.025) and induced a significant 17.7% decrease in the athletes' muscular power (p=0.030).CONCLUSIONS:This study shows the negative impacts of an occlusal disturbance on the athletic performance of young elite rowers. The detection of malocclusion traits by regular occlusal monitoring would be of great interest in this population.
The immunoreactivity of the gadolinium (Gd)-labeled anti-CEA F(ab')2 immunoconjugates was 80% to 85%. Compared with that of commercial chelates, the relaxivity (R1) increase is as follows: Gd-DTPA < Gd-DOTA < Gd-H2O < PL-Gd-DTPA24-28 < PL-Gd-DTPA24-28 F(ab')2 < PL-Gd-DOTA24-28 < PL-Gd-DOTA24-28 F(ab')2. 1H nuclear magnetic relaxation dispersion data of immunoconjugates showed that the high relaxivity enhancement was the result of a reduction of the molecular tumbling rate. Twenty-four hours after intravenous injection of 50 micrograms (1 mumol Gd/kg) of Gd-labeled immunoconjugates to nude mice grafted with human colorectal carcinoma LS 174T, the tumor uptake was 10% to 15%, resulting in an increase of R1 of up to 15% to 20% versus noninjected mice. No difference was found between PL-Gd-DTPA24-28 F(ab')2 and PL-Gd-DOTA24-28 F(ab')2 immunoconjugates for tumor, liver, and kidney uptake. A high signal intensity of tumor was observed in 50% of the tested mice.
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