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Title: Nitrile regio-synthesis by Ni centers on a siliceous surface: implications in prebiotic chemistry
By means of quantum chemistry (PBE0/def2-TZVPP; DLPNO-CCSD(T)/cc-pVTZ) and small, but reliable models of Polyhedral Oligomeric Silsesquioxanes (POSS), an array of astrochemically-relevant catalysis products, related to prebiotic and origin of life chemistry, has been theoretically explored. In this work, the heterogeneous phase hydrocyanation reaction of an unsaturated CC bond (propene) catalyzed by a Ni center complexed to a silica surface is analyzed. Of the two possible regioisomers, the branched iso-propyl-cyanide is thermodynamically and kinetically preferred over the linear n -propyl-cyanide ( T = 200 K). The formation of nitriles based on a regioselective process has profound implications on prebiotic and origin of life chemistry, as well as deep connections to terrestrial surface chemistry and geochemistry.  more » « less
Award ID(s):
1846408
NSF-PAR ID:
10431074
Author(s) / Creator(s):
;
Date Published:
Journal Name:
Chemical Communications
Volume:
58
Issue:
82
ISSN:
1359-7345
Page Range / eLocation ID:
11579 to 11582
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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