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Metal-Ion- and Hydrogen-Bond-Mediated Interstellar Prebiotic Chemistry: The First Step in the Formose Reaction.
Journal of Physical Chemistry. A 2017 November 17
The formose reaction, which offers a feasible chemical pathway for the prebiotic synthesis of sugars, is a well-studied reaction for over two hundred and 50 years. Yet huge knowledge gaps exist even in the very first step of the formose reaction. In this work, we provide a new and otherwise unintuitive reaction pathway for the gas-phase conversion of formaldehyde to glycolaldehyde (the first step in the formose reaction) occurring in the interstellar medium (ISM). Employing electronic structure calculations (CCSD(T) and DFT methods), we exhaustively probe the role of various metal ions and small molecules detected in the ISM to propose a new mechanism wherein metal-oxygen interactions and hydrogen bonds cooperatively facilitate an otherwise implausible chemical reaction. The reactions involving Mg2+ are throughout found to be barrierless, and those featuring Al+ ions are noted to only have a small barrier. The proton affinities of the small molecules, metal-oxygen interactions, and the extent of C-C-bond formation are found to be the significant factors that influence the barrier heights. The mechanism is also shown to be consistent with well-known experimental details in the terrestrial formose reaction (which could, however, proceed through a different mechanism). Future experimental and theoretical scope arising out of this paper are subsequently discussed.
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