Deutérium

Résumé

Le deutérium, noté H ou D, est l'isotope de l'hydrogène dont le nombre de masse est égal à 2 : son noyau atomique, appelé deuton ou deutéron, compte et avec un spin 1+ pour une masse atomique de . Il est caractérisé par un excès de masse de et une énergie de liaison nucléaire par nucléon de . Il s'agit d'un isotope stable découvert en 1931 par Harold Clayton Urey, chimiste à l'université Columbia ; cette découverte lui valut le prix Nobel de chimie en 1934. vignette|Tube à gaz au deutérium. Différences entre protium et deutérium Symbole chimique L'UICPA recommande de représenter le deutérium par le symbole H afin de préserver l'homogénéité de ses dénominations, mais tolère le symbole D qui est largement utilisé. La raison de cette tolérance serait à chercher dans le fait que, de tous les éléments chimiques, l'hydrogène est celui pour lequel les isotopes ont des différences de masse relatives les plus élevées. Cela a des conséquen

Source officielle

https://fr.wikipedia.org/wiki/Deut%C3%A9rium

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Nuclear magnetic resonance (NMR) spectroscopy is one of the most powerful and informative methods to probe molecular dynamics. Specifically, chemical exchange is an important phenomenon and one of the earliest and most vigorously investigated in NMR spectroscopy. Its effects can be observed in many NMR spectra; lines in a spectrum are broadened or averaged because the nuclei are exchanging magnetic environments. A wide variety of experimental methods exists to determine exchange rates of protons that hop between amino acids and water in the slow or intermediate exchange regime. However, so far there is a lack of methods to investigate hydrogen exchange in the fast exchange regime. In this thesis, we focus on the determination of very fast chemical exchange rates from the effects of scalar relaxation on a coupled nucleus. We quantify the effects of scalar relaxation caused by exchanging hydrogens, by detecting the decay of a 15N coherence under a multiple-refocusing Carr-Purcell-Meiboom-Gill (CPMG) pulse train in the presence or absence of hydrogen decoupling. In particular, we have adapted to the case of deuterium a method that was originally designed to study the exchange rate of the indole proton of tryptophan in water as a function of pH and temperature. We will present the exchange rates of the indole deuterium in tryptophan with solvent heavy water. After that, the proton exchanges rates have been compared with the deuterium exchange rates in order to describe the kinetic isotope effect. In a similar manner, we have quantified the proton exchange rates in pure water by using multiple refocusing of transverse 17O magnetization as a function of pH and temperature. Such measurements are widely used to obtain valuable information about molecular dynamics and structure of proteins, protein complexes and nucleic acids. The knowledge of the kinetic isotope effect may contribute to the characterization of reaction mechanisms and other dynamic parameters that can give insight into the stability of hydrogen bonded secondary structures in biomolecules. This information could form a foundation for a more thorough theoretical or modeling development of a number of long and outstanding fundamental questions. In the second part of the thesis, we combine fast exchange with dissolution dynamic nuclear polarization (D-DNP) to study intrinsically disordered proteins (IDPs). IDPs constitute a very large and functionally important class of proteins that lack stable secondary and tertiary structures. As a consequence of the broad dynamics and flexibility of IDPs, and specially under physiological conditions, the NMR spectra of IDPs typically show a strong signal overlap and broadening due to proton exchange. We present a method to overcome these limitations by means of hyperpolarized HDO produced by D-DNP. We could study the effects of conformational adaptations in Osteopontin (OPN), a metastasis- associated intrinsically disordered protein (IDP) by chemical exchange. The magnetization from hyperpolarized water is transferred to the rapidly exchanging protons of the solvent-exposed residues of the protein. The exchange with hyperpolarized water boosts the signals of fast exchanging residues above the detection limits. This allows one to follow individual resonances and draw conclusions regarding conformational adaptations due to ligand binding under physiological conditions. Thus, with our approach, exchange with the solvent is turned into an advantage

EPFL2017

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Kinetic isotope effects for fast deuterium and proton exchange rates

Geoffrey Bodenhausen, Estel Canet Martinez, Pavel Kaderavek, Daniele Mammoli

By monitoring the effect of deuterium decoupling on the decay of transverse N-15 magnetization in D-N-15 spin pairs during multiple-refocusing echo sequences, we have determined fast D-D exchange rates k(D) and compared them with fast H-H exchange rates k(H) in tryptophan to determine the kinetic isotope effect as a function of pH and temperature.

Royal Society of Chemistry2016

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NanoSIMS analysis of organic carbon from the Tissint Martian meteorite: Evidence for the past existence of subsurface organic-bearing fluids on Mars

Philippe Gillet, Lin Xu, Wei Yang, Jing Yang

Two petrographic settings of carbonaceous components, mainly filling open fractures and occasionally enclosed in shock-melt veins, were found in the recently fallen Tissint Martian meteorite. The presence in shock-melt veins and the deuterium enrichments (delta D up to +1183 parts per thousand) of these components clearly indicate a pristine Martian origin. The carbonaceous components are kerogen-like, based on micro-Raman spectra and multielemental ratios, and were probably deposited from fluids in shock-induced fractures in the parent rock of Tissint. After precipitation of the organic matter, the rock experienced another severe shock event, producing the melt veins that encapsulated a part of the organic matter. The C isotopic compositions of the organic matter (delta C-13 = -12.8 to -33.1 parts per thousand) are significantly lighter than Martian atmospheric CO2 and carbonate, providing a tantalizing hint for a possible biotic process. Alternatively, the organic matter could be derived from carbonaceous chondrites, as insoluble organic matter from the latter has similar chemical and isotopic compositions. The presence of organic-rich fluids that infiltrated rocks near the surface of Mars has significant implications for the study of Martian paleoenvironment and perhaps to search for possible ancient biological activities on Mars.

Wiley-Blackwell2014

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EPFL2017