TY - JOUR

T1 - Chemical Analysis of a “Miller-Type” Complex Prebiotic Broth

T2 - Part II: Gas, Oil, Water and the Oil/Water-Interface

AU - Scherer, Sabrina

AU - Wollrab, Eva

AU - Codutti, Luca

AU - Carlomagno, Teresa

AU - da Costa, Stefan Gomes

AU - Volkmer, Andreas

AU - Bronja, Amela

AU - Schmitz, Oliver J.

AU - Ott, Albrecht

N1 - Publisher Copyright: © 2016, The Author(s). Copyright: Copyright 2017 Elsevier B.V., All rights reserved.

PY - 2017/12

Y1 - 2017/12

N2 - We have analyzed the chemical variety obtained by Miller-Urey-type experiments using nuclear magnetic resonance (NMR) spectroscopy and coherent anti-Stokes Raman scattering (CARS) spectroscopy, gas chromatography followed by mass spectrometry (GC/MS) and two-dimensional gas chromatography followed by mass spectrometry (GCxGC/MS). In the course of a running Miller-Urey-type experiment, a hydrophobic organic layer emerged besides the hydrophilic aqueous phase and the gaseous phase that were initially present. The gas phase mainly consisted of aromatic compounds and molecules containing C≡C or C≡N triple bonds. The hydrophilic phase contained at least a few thousands of different molecules, primarily distributed in a range of 50 and 500 Da. The hydrophobic phase is characterized by carbon-rich, oil-like compounds and their amphiphilic derivatives containing oxygen with tensioactive properties. The presence of a wide range of oxidized molecules hints to the availability of oxygen radicals. We suggest that they intervene in the formation of alkylated polyethylene glycol (PEG) in the oil/water interface. CARS spectroscopy revealed distinct vibrational molecular signatures. In particular, characteristic spectral bands for cyanide compounds were observed if the broth was prepared with electric discharges in the gaseous phase. The characteristic spectral bands were absent if discharges were released onto the water surface. NMR spectroscopy on the same set of samples independently confirmed the observation. In addition, NMR spectroscopy revealed overall high chemical variability that suggests strong non-linearities due to interdependent, sequential reaction steps.

AB - We have analyzed the chemical variety obtained by Miller-Urey-type experiments using nuclear magnetic resonance (NMR) spectroscopy and coherent anti-Stokes Raman scattering (CARS) spectroscopy, gas chromatography followed by mass spectrometry (GC/MS) and two-dimensional gas chromatography followed by mass spectrometry (GCxGC/MS). In the course of a running Miller-Urey-type experiment, a hydrophobic organic layer emerged besides the hydrophilic aqueous phase and the gaseous phase that were initially present. The gas phase mainly consisted of aromatic compounds and molecules containing C≡C or C≡N triple bonds. The hydrophilic phase contained at least a few thousands of different molecules, primarily distributed in a range of 50 and 500 Da. The hydrophobic phase is characterized by carbon-rich, oil-like compounds and their amphiphilic derivatives containing oxygen with tensioactive properties. The presence of a wide range of oxidized molecules hints to the availability of oxygen radicals. We suggest that they intervene in the formation of alkylated polyethylene glycol (PEG) in the oil/water interface. CARS spectroscopy revealed distinct vibrational molecular signatures. In particular, characteristic spectral bands for cyanide compounds were observed if the broth was prepared with electric discharges in the gaseous phase. The characteristic spectral bands were absent if discharges were released onto the water surface. NMR spectroscopy on the same set of samples independently confirmed the observation. In addition, NMR spectroscopy revealed overall high chemical variability that suggests strong non-linearities due to interdependent, sequential reaction steps.

KW - coherent anti-Stokes Raman scattering (CARS)

KW - Complex chemical mixture

KW - GC/MS

KW - GCxGC/MS

KW - Miller-Urey experiment

KW - Molecular vibrations

KW - NMR

KW - Oil/water interface

KW - Origin of Life

KW - Phase-transfer-catalysis

KW - Radicals

UR - http://www.scopus.com/inward/record.url?scp=84997701852&partnerID=8YFLogxK

U2 - 10.1007/s11084-016-9528-8

DO - 10.1007/s11084-016-9528-8

M3 - Article

C2 - 27896547

AN - SCOPUS:84997701852

VL - 47

SP - 381

EP - 403

JO - Origins of Life and Evolution of Biospheres

JF - Origins of Life and Evolution of Biospheres

SN - 0169-6149

ER -