On the origin and evolution of deuterium enrichment in type 1 and 2 chondritic organic solids

Rotationally resonant Deuterium Nuclear Magnetic Resonance spectroscopy (D MAS NMR) was applied to IOM isolated from a CR1 chondrite Grosvenor Mountains (GRO) 95577 and a CM2 chondrite (Murchison). It is shown that in IOM D strongly prefers the aliphatic hydrogen reservoir over the aromatic hydrogen reservoir. For GRO 95577, that has a bulk δD of 3303 ‰ (Alexander et al., 2010), the average δD value of the aromatic reservoir is 1740 ± 128 ‰ and the aliphatic reservoir is 4477 ± 105 ‰, i.e., D/H enrichments of 1.27 and 0.64, respectively, relative to the bulk. For Murchison IOM, that has a bulk δD of 811 ‰ (Alexander et al., 2010), the average δD of the aromatic reservoir is 512 ± 88 ‰ and the aliphatic reservoir is 1033 ± 64 ‰ i.e., D/H enrichments of 1.12 and 0.82, respectively, relative to the bulk. D-H exchange between D-enriched water and a type III kerogen reveals nearly equivalent D up take by both aromatics and aliphatics. Laboratory synthesis of IOM-like material in the presence of D₂O reveals a high degree of deuteration with a strong preferential deuteration of the aliphatic hydrogen reservoir indicating that the δD of the water during IOM synthesis is the primary determinant of syn-IOM’s δD. The IOM in GRO 95577 and Murchison (FA and H/C × 100) lie on the molecular evolution line as defined by the IOM of the Tagish Lake clasts and Murchison IOM has experienced more molecular evolution relative to that exhibited by GRO 95577 IOM. A forward prediction derived from the D/H ratios for the aliphatic and aromatic hydrogen reservoirs in Murchison and GRO 95577, relative to their bulk D/H ratios, derived from D MAS NMR, is applied to explain the origin of the Tagish Lake trend of δD vs molecular evolution (H/C × 100). The results of this forward prediction suggest that the Tagish Lake isotopic trend results from a combination of molecular evolution (loss of predominantly aliphatic H and D) and partial D-H exchange with D depleted chondritic water during a short-term hydrothermal alteration event. Such events may be faithfully identified in chondritic organic solids and be a common occurrence, but not necessarily revealed in the mineralogy of type 1 and 2 carbonaceous chondrites.