Universität zu Köln

Niether, Doreen ORCID: 0000-0002-8496-4215, Afanasenkau, Dzmitry, Dhont, Jan K. G. and Wiegand, Simone ORCID: 0000-0001-6333-1956 (2016). Accumulation of formamide in hydrothermal pores to form prebiotic nucleobases. Proc. Natl. Acad. Sci. U. S. A., 113 (16). S. 4272 - 4278. WASHINGTON: NATL ACAD SCIENCES. ISSN 0027-8424

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Abstract

Formamide is one of the important compounds from which prebiotic molecules can be synthesized, provided that its concentration is sufficiently high. For nucleotides and short DNA strands, it has been shown that a high degree of accumulation in hydrothermal pores occurs, so that temperature gradients might play a role in the origin of life [ Baaske P, et al. (2007) Proc Natl Acad Sci USA 104(22): 9346-9351]. We show that the same combination of thermophoresis and convection in hydrothermal pores leads to accumulation of formamide up to concentrations where nucleobases are formed. The thermophoretic properties of aqueous formamide solutions are studied by means of Infrared Thermal Diffusion Forced Rayleigh Scattering. These data are used in numerical finite element calculations in hydrothermal pores for various initial concentrations, ambient temperatures, and pore sizes. The high degree of formamide accumulation is due to an unusual temperature and concentration dependence of the thermophoretic behavior of formamide. The accumulation fold in part of the pores increases strongly with increasing aspect ratio of the pores, and saturates to highly concentrated aqueous formamide solutions of similar to 85 wt% at large aspect ratios. Time-dependent studies show that these high concentrations are reached after 45-90 d, starting with an initial formamide weight fraction of 10(-3) wt % that is typical for concentrations in shallow lakes on early Earth.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Niether, Doreen UNSPECIFIED orcid.org/0000-0002-8496-4215 UNSPECIFIED Afanasenkau, Dzmitry UNSPECIFIED UNSPECIFIED UNSPECIFIED Dhont, Jan K. G. UNSPECIFIED UNSPECIFIED UNSPECIFIED Wiegand, Simone UNSPECIFIED orcid.org/0000-0001-6333-1956 UNSPECIFIED
URN:	urn:nbn:de:hbz:38-278510
DOI:	10.1073/pnas.1600275113
Journal or Publication Title:	Proc. Natl. Acad. Sci. U. S. A.
Volume:	113
Number:	16
Page Range:	S. 4272 - 4278
Date:	2016
Publisher:	NATL ACAD SCIENCES
Place of Publication:	WASHINGTON
ISSN:	0027-8424
Language:	English
Faculty:	Faculty of Mathematics and Natural Sciences
Divisions:	Faculty of Mathematics and Natural Sciences > Department of Chemistry > Institute of Physical Chemistry
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language MOLECULAR-DYNAMICS SIMULATION; ETHANOL-WATER MIXTURES; THERMAL-DIFFUSION; SORET COEFFICIENT; AQUEOUS-SOLUTIONS; HYDROGEN-CYANIDE; TEMPERATURE-DEPENDENCE; COLLOIDAL SUSPENSIONS; CHARGED COLLOIDS; AMINO-ACIDS Multiple languages Multidisciplinary Sciences Multiple languages
Refereed:	Yes
URI:	http://kups.ub.uni-koeln.de/id/eprint/27851