Isotope record of mineralogical changes in a spectrum of aqueously altered CM chondrites

Elishevah M.M.E. van Kooten, Larissa L. Cavalcante, Kazuhide Nagashima, Takeshi Kasama, Zoltan I. Balogh, Zan Peeters, Silver Sung-Yun Hsiao, Hsien Shang, Der-Chuen Lee, Typhoon Lee, Alexander N. Krot, Martin Bizzarro

Geochimica et Cosmochimica Acta
Available online 25 June 2018

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“The recent fall of the relatively unaltered CM chondrite Maribo provides a unique opportunity to study the early stages of aqueous alteration on the CM chondrite parent body. We show using transmission electron microscopy of a matrix FIB-section from Maribo that this meteorite mainly appears to consist of tochilinite-cronstedtite intergrowths (TCIs), but also contains regions of amorphous or nanocrystalline silicates, anhydrous silicates and FeNi metal aggregates with thin iron oxide rims, suggesting that it experienced aqueous alteration to a relatively small degree. A comparison of Maribo with increasingly altered CM chondrites such as Jbilet Winselwan and Bells shows that during progressive aqueous alteration (1) the TCIs are replaced by coarser sulfides and increasingly Mg-rich serpentine, and (2) the abundance of 1515N-rich hotspots increases, whereas the magnitude of their 1515N enrichment decreases. We observe that the overall N isotope variability related to aqueous alteration is an order of magnitude lower than the variability observed between different chondrite groups. We suggest these high order differences are the result of heterogeneous accretion of insoluble or soluble organic carriers of 1515N to the different chondrite parent bodies. D/H ratios of matrices from Maribo, Jbilet Winselwan and Bells increase with progressive aqueous alteration, a trend that is opposite to expectations of mixing between D-poor water and D-rich organic matter. We argue that this behaviour cannot be related to Fe oxidation or serpentinization reactions and subsequent loss of D-poor H2 gas. We offer an alternative hypothesis and suggest that CM chondrites experienced two-stage aqueous alteration. During the first stage occurring at relatively low temperature, mixing of increasing amounts of D-poor water with D-rich organic matter results in a decrease of D/H ratio with increasing degree of alteration. During the second stage of alteration occurring at relatively high temperature (T << 300 °°C), decomposition of TCIs in CMs of petrologic type <<2.7 releases gaseous D-poor water that results in increase of the D/H ratio of the CM matrices. Finally, we report on changes in the organic structure of Maribo, Jbilet Winselwan and Bells using Carbon-K and Nitrogen-K edge electron energy loss spectroscopy. The organic matter initially has higher aromatic/aliphatic ratios (e.g., Maribo) and lower abundances of ketone and carboxyl functional groups, which we suggest are the result of chemical degradation of double bonded carbon from oxidation during hydrothermal alteration. Consequently, we propose that the organic matter of the CM chondrite Paris, for which lower aromatic/aliphatic ratios have been observed, may have been different from Maribo, perhaps reflecting the early accretion of Paris relative to Maribo."