Solid-state (1H and 13C) nuclear magnetic resonance spectroscopy of insoluble organic residue in the Murchison meteorite:: A self-consistent quantitative analysis

被引:179
作者
Cody, GD
Alexander, CMO
Tera, F
机构
[1] Carnegie Inst Washington, Geophys Lab, Washington, DC 20015 USA
[2] Carnegie Inst Washington, Dept Terr Magnetism, Washington, DC 20015 USA
基金
美国国家科学基金会;
关键词
D O I
10.1016/S0016-7037(01)00888-2
中图分类号
P3 [地球物理学]; P59 [地球化学];
学科分类号
0708 ; 070902 ;
摘要
Complementary, double- and single-resonance solid-state (H-1 and C-13) nuclear magnetic resonance (NMR) experiments were performed on a solvent extracted and demineralized sample of Murchison meteorite organic macromolecule. These NMR data provide a consistent picture of a complex organic solid composed of a wide range of organic (aromatic and aliphatic) functional groups, including numerous oxygen-containing functional groups. The fraction of aromatic carbon within the Murchison organic residue (constrained by three independent experiments) lies between 0.61 and 0.66. The close similarity in cross-polarized and single-pulse spectra suggests that both methods detect the same distribution of carbon. With the exception of interstellar diamond (readily detected in slow magic angle spinning single-pulse NMR experiments), there is no evidence in the solid-state NMR data for a significant abundance of large laterally condensed aromatic molecules in the Murchison organic insoluble residue. Given the most optimistic estimation, such carbon would not exceed 10%, and more likely is a fraction of this maximum estimate. The fraction of aromatic carbon directly bonded to hydrogen is low (similar to30%), indicating that the aromatic molecules in the Murchison organic residue are highly substituted. The bulk hydrogen content, H/C, derived from NMR data, ranges from a low of 0.53 +/- 0.06 and a high of 0.63 +/- 0.06. The hydrogen content (H/C) determined via elemental analysis is 0.53. The range of oxygen-containing organic functionality in the Murchison is substantial. Depending on whether various oxygen-containing organic functional groups exist as free acids and hydroxyls or are linked as esters and ethers results in a wide range in O/C (0.22 to 0.37). The lowest values are more consistent with elemental analyses, requiring that oxygen-containing functional groups in the Murchison macromolecule are highly linked. The combined H-1 and C-13 NMR data reveal a high proportion of methine carbon, which requires that carbon chains within the Murchison organic macromolecule are highly branched. Copyright (C) 2002 Elsevier Science Ltd.
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页码:1851 / 1865
页数:15
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