Journal
INORGANIC CHEMISTRY
Volume 51, Issue 6, Pages 3883-3890Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ic3000944
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Funding
- National Science Foundation [DMR- 0348982]
- U.S. Department of Energy (DOE) [DE-FG02-05ER15736]
- NSF-East Asia-Pacific Summer Institute (EAPSI)
- Japan Society for The Promotion of Science (JSPS)
- U.S. Department of Energy (DOE) [DE-FG02-05ER15736] Funding Source: U.S. Department of Energy (DOE)
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We have investigated the assembly of a two-dimensional coordination polymer, Nd-2(C6H2N2O4)(2)(C2O4)-(H2O)(2), that has been prepared from the hydrothermal reaction of Nd(NO3)(3)center dot 6H(2)O and 2,3-pyrazinedicarboxylic acid (H(2)pzdc). In situ oxalate formation as observed in this system has been been investigated using H-1 and C-13 nuclear magnetic resonance spectroscopy, and a pathway for C2O42- anion formation under hydrothermal conditions has been elucidated. The oxalate ligands found in Nd-2(C6H2N2O4)(2)(C2O4)(H2O)(2) result from the oxidation of H(2)pzdc, which proceeds through intermediates, such as 2-pyrazinecarboxylic acid (2-pzca), 2-hydroxyacetamide, 3-amino-2-hydroxy-3-oxopropanoic acid, 2-hydroxymalonic acid, 2-oxoacetic acid (glyoxylic acid), and glycolic acid. The species are generated through a ring-opening that occurs via cleavage of the C-N bond of the pyrazine ring, followed by hydrolysis/oxidation of the resulting species.
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