Structure and isotopic ratios of aliphatic side chains in the insoluble organic matter of the Murchison carbonaceous chondrite

被引:40
作者
Huang, Yongsong [1 ]
Alexandre, Marcelo R. [1 ]
Wang, Yi [1 ]
机构
[1] Brown Univ, Dept Geol Sci, Providence, RI 02912 USA
基金
美国国家航空航天局;
关键词
Murchison; carbonaceous chondrite; RuO4; oxidation; SPME; aliphatic side chain;
D O I
10.1016/j.epsl.2007.05.012
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
We report in this paper the first molecular and isotopic characterization of individual aliphatic side chains from the insoluble organic matter (IOM) in the Murchison carbonaceous chondrite using a novel combined approach of RUO4 oxidation and solid phase microextraction (SPME). The aliphatic side chains in the IOM of Murchison were first released by oxidizing aromatic structures using RUO4. Because the IOM of carbonaceous chondrites contains predominantly short (C-1 to C-9) aliphatic substitutions. the resulting low molecular weight monocarboxylic acids (MCAs) are highly volatile and water-soluble. The conventional aqueous extraction and derivatization procedures following RUO4 oxidation are unable to recover MCAs for subsequent analyses. We overcame this problem by employing SPME to directly capture the MCAs from the aqueous solution. We selected a SPME fiber with greater affinity for longer chain monoacids to compensate for the exponential decline of monoacid concentrations with increasing carbon numbers in meteorite IOM, allowing more accurate identification and quantification for the less abundant monoacids. We also determined the carbon and hydrogen isotopic ratios of individual MCAs derived from Murchinson IOM. Our results reveal significant similarity in both molecular structures and hydrogen isotopic ratios between the IOM aliphatic side chains and water-soluble MCAs in Murchison, suggesting that these compounds had common precursors. Our combined new approach of RuO4 oxidation-SPME provides a new way to probe the molecular and isotopic characteristics of aliphatic side chains in carbonaceous chondrites. (c) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:517 / 525
页数:9
相关论文
共 35 条
[21]  
Ng LK, 1996, J SCI FOOD AGR, V70, P380, DOI 10.1002/(SICI)1097-0010(199603)70:3<380::AID-JSFA517>3.0.CO
[22]  
2-M
[23]   Solid-phase microextraction coupled to gas chromatography/mass spectrometry for determining polycyclic aromatic hydrocarbon-micelle partition coefficients [J].
Pino, V ;
Ayala, JH ;
González, V ;
Afonso, AM .
ANALYTICAL CHEMISTRY, 2004, 76 (15) :4572-4578
[24]   The chemistry of life's origin: A carbonaceous meteorite perspective [J].
Pizzarello, S .
ACCOUNTS OF CHEMICAL RESEARCH, 2006, 39 (04) :231-237
[25]   The deuterium enrichment of individual amino acids in carbonaceous meteorites: A case for the presolar distribution of biomolecule precursors [J].
Pizzarello, S ;
Huang, YS .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2005, 69 (03) :599-605
[26]   Nonracemic isovaline in the Murchison meteorite: Chiral distribution and mineral association [J].
Pizzarello, S ;
Zolensky, M ;
Turk, KA .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2003, 67 (08) :1589-1595
[27]   New pyrolytic and spectroscopic data on Orgueil and Murchison insoluble organic matter: A different origin than soluble? [J].
Remusat, L ;
Derenne, S ;
Robert, F ;
Knicker, H .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2005, 69 (15) :3919-3932
[28]   New insight on aliphatic linkages in the macromolecular organic fraction of Orgueil and Murchison meteorites through ruthenium tetroxide oxidation [J].
Remusat, L ;
Derenne, S ;
Robert, F .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2005, 69 (17) :4377-4386
[29]  
ROBERT F, 1982, GEOCHIM COSMOCHIM AC, V46, P81, DOI 10.1016/0016-7037(82)90293-9
[30]   Investigating the variations in carbon and nitrogen isotopes in carbonaceous chondrites [J].
Sephton, MA ;
Verchovsky, AB ;
Bland, PA ;
Gilmour, I ;
Grady, MM ;
Wright, IP .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2003, 67 (11) :2093-2108