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Chemical Transformations in Proto-Cytoplasmic Media. Phosphorus Coupling in the Silica Hydrogel Phase

School of Chemistry, University of Leeds, Woodhouse Lane, Leeds LS2 9JT, UK
Author to whom correspondence should be addressed.
Received: 7 August 2017 / Revised: 12 October 2017 / Accepted: 27 October 2017 / Published: 19 November 2017
(This article belongs to the Special Issue Phosphorus (P) and the Origins of Life)
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It has been proposed that prebiotic chemical studies on the emergence of primitive life would be most relevant when performed in a hydrogel, rather than an aqueous, environment. In this paper we describe the ambient temperature coupling of phosphorus oxyacids [Pi] mediated by Fe(II) under aerobic conditions within a silica hydrogel (SHG) environment. We have chosen to examine SHGs as they have considerable geological precedence as key phases in silicification en route to rock formation. Following a description of the preparation and characterization studies on our SHG formulations, coupling experiments between Pi species are described across multiple permutations of (i) Pi compound; (ii) gel formulation; (iii) metal salt additive; and (iv) pH-modifying agent. The results suggest that successful Pi coupling, indicated by observation of pyrophosphate [PPi(V)] via 31P-NMR spectroscopy, takes place when the following components are present: (i) a mixture of mixture of Pi(III) and Pi(V) or pure PPi(III-V); (ii) Fe(II); (iii) acetic or formic acid (not hydrochloric acid); (iv) aerobic conditions or the presence of H2O2 as an oxidant; and (v) the presence of a gel system. On the basis of these, and aqueous control reactions, we suggest mechanistic possibilities. View Full-Text
Keywords: silica; hydrogel; phosphorus; coupling; prebiotic silica; hydrogel; phosphorus; coupling; prebiotic

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Gorrell, I.B.; Henderson, T.W.; Albdeery, K.; Savage, P.M.; Kee, T.P. Chemical Transformations in Proto-Cytoplasmic Media. Phosphorus Coupling in the Silica Hydrogel Phase. Life 2017, 7, 45.

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