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• W15826306 abstract "Introduction: One of the hallmark properties of primitive organic solids (IOM) in type 1 & 2 chondrites is the high deuterium content relative to Galactic and Solar values [1]. The high D enrichment in IOM has largely been attributed to small molecule chemistry that occurred, prior to the synthesis of IOM, in the InterStellar Medium (ISM) at very low temperatures where extensive fractionation can occur through ionmolecule reactions (predominantly reactions with H2D and CH2D). The potential for heavy D enrichment is revealed through the detection of highly deuterated formaldehyde and methanol with D/H ratios up to 10 [2]. Extremely D enriched formaldehyde and methanol (up to D2CO and CD3OH) have also been observed in the early “hot corino” stage of molecular cloud collapse and early Solar System formation [3]. Placing these very high D enrichments in context, it is noteworthy that even highly D enriched chondritic IOM, e.g. the CR1 chondrite GRO95577 [4] with a bulk δD of 3235 ‰, is only slightly enriched relative to terrestrial water (by a factor of ~ 4 x). Thus, while isotopically IOM is exotic relative to terrestrial D/H, it is by no means close to the enrichments observed for small molecules in the ISM and cold molecular clouds. This fact has been recognized by others [5], who proposed that previously formed IOM (by an unstated mechanism) initially has a very low D/H but was enriched in D in the outer regions of the Solar System at temperatures on the order of 120 K, via D-H exchange of IOM with H2D. It was further proposed that different bonds will exchange D with H at rates proportional to their bond strength, thus benzylic carbon was predicted to be isotopically heavier then aliphatic carbon that is predicted to be isotopically heavier than aromatic H. In the case of IOM derived from Orgueil (CI1) it was concluded that for benyzlic carbon δD = 1250‰, aliphatic carbon δD =550‰, and aromatic carbon δD =150‰. Direct detection of deuterium substitution via solid-state H NMR provides an unambiguous means of assessing whether there exists any detectible difference in D abundance amongst organic functional groups. The problem is that natural abundance H NMR is one of the least sensitive NMR experiments, e.g. for terrestrial values of D, the sensitivity of H NMR is 1.45 x 10 that of H NMR. Furthermore, H NMR spectra are complicated by the fact that deuterium is a spin 1 quadrupole, which means that the spectrum appears as a series of rotational echos spread out over the frequency range of the quadrupole interaction, up to 140 Khz for D in rigid environments. Notwithstanding this difficulty we have developed an experimental protocol that allows us to obtain purely isotropic H NMR spectra, devoid of the quadrupolar artifacts. We can then compare these spectra with H NMR spectra to assess the local variation in D enrichment. It should be noted that the frequency distribution of D-functional groups in H NMR spectra are nearly identical with the distribution of H-functional groups in H NMR spectra, with the exception of a small frequency shift associated with the scalar quadrupolar shift." @default.
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• W15826306 date "2011-03-01" @default.
• W15826306 modified "2023-09-23" @default.
• W15826306 title "Deuterium Speciation in Chondritic Organic Solids: A Relic of Cold Molecular Processes" @default.
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