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J. Biol. Chem., Vol. 282, Issue 23, 16729-16735, June 8, 2007

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Nucleoside Phosphorylation by Phosphate Minerals^*

Giovanna Costanzo, Raffaele Saladino, Claudia Crestini^¶, Fabiana Ciciriello^||, and Ernesto Di Mauro^||1

From the Istituto di Biologia e Patologia Molecolari, Consiglio Nazionale delle Ricerche, Pizalle Aldo Moro, 5, 00185 Rome, Italy, Dipartimento AgroBiologia and AgroChimica, Università della Tuscia, Via San Camillo De Lellis, 01100 Viterbo, Italy, ^¶Dipartimento di Scienze e Tecnologie Chimiche, Università "Tor Vergata", 00133 Rome, Italy, and ^||Dipartimento di Genetica e Biologia Molecolare, Fondazione "Istituto Pasteur-Fondazione Cenci-Bolognetti" Università "La Sapienza" di Roma, Pizalle Aldo Moro, 5, 00185 Rome, Italy

In the presence of formamide, crystal phosphate minerals may act as phosphate donors to nucleosides, yielding both 5'- and, to a lesser extent, 3'-phosphorylated forms. With the mineral Libethenite the formation of 5'-AMP can be as high as 6% of the adenosine input and last for at least 10³ h. At high concentrations, soluble non-mineral phosphate donors (KH₂PO₄ or 5'-CMP) afford 2'- and 2':3'-cyclic AMP in addition to 5'-and 3'-AMP. The phosphate minerals analyzed were Herderite Ca[BePO₄F], Hureaulite Mn²⁺₅(PO₃(OH)₂(PO₄)₂(H₂O)₄, Libethenite Cu²⁺₂(PO₄)(OH), Pyromorphite Pb₅(PO₄)₃Cl, Turquoise Cu²⁺Al₆(PO₄)₄(OH)₈(H₂O)₄, Fluorapatite Ca₅(PO₄)₃F, Hydroxylapatite Ca₅(PO₄)₃OH, Vivianite Fe²⁺₃(PO₄)₂(H₂O)₈, Cornetite Cu²⁺₃(PO₄)(OH)₃, Pseudomalachite Cu²⁺₅(PO₄)₂(OH)₄, Reichenbachite Cu²⁺₅(PO₄)₂(OH)₄, and Ludjibaite Cu²⁺₅(PO₄)₂(OH)₄). Based on their behavior in the formamide-driven nucleoside phosphorylation reaction, these minerals can be characterized as: 1) inactive, 2) low level phosphorylating agents, or 3) active phosphorylating agents. Instances were detected (Libethenite and Hydroxylapatite) in which phosphorylation occurs on the mineral surface, followed by release of the phosphorylated compounds. Libethenite and Cornetite markedly protect the -glycosidic bond. Thus, activated nucleic monomers can form in a liquid non-aqueous environment in conditions compatible with the thermodynamics of polymerization, providing a solution to the standard-state Gibbs free energy change (G°') problem, the major obstacle for polymerizations in the liquid phase in plausible prebiotic scenarios.

Received for publication, December 11, 2006 , and in revised form, April 3, 2007.

^* This work was supported by the Italian Space Agency Project MoMa and Centro di Eccellenza di Biologia e Medicina Molecolare, Università "La Sapienza". The costs of publication of this article were defrayed in part by the payment of page charges. This article must therefore be hereby marked "advertisement" in accordance with 18 U.S.C. Section 1734 solely to indicate this fact.

¹ To whom correspondence should be addressed. Tel.: 39-06-49912880; Fax: 39-06-49912500; E-mail: Ernesto.dimauro{at}uniroma1.it.

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