Investigation of in Situ Oxalate Formation from 2,3-Pyrazinedicarboxylate under Hydrothermal Conditions Using Nuclear Magnetic Resonance Spectroscopy

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• 作者：Karah E. Knope ; Hiroshi Kimura ; Yoshiro Yasaka ; Masaru Nakahara ; Michael B. Andrews ; Christopher L. Cahill
• 刊名：Inorganic Chemistry
• 出版年：2012
• 出版时间：March 19, 2012
• 年：2012
• 卷：51
• 期：6
• 页码：3883-3890
• 全文大小：389K
• 年卷期：v.51,no.6(March 19, 2012)
• ISSN：1520-510X

文摘

We have investigated the assembly of a two-dimensional coordination polymer, Nd₂(C₆H₂N₂O₄)₂(C₂O₄)(H₂O)₂, that has been prepared from the hydrothermal reaction of Nd(NO₃)₃路6H₂O and 2,3-pyrazinedicarboxylic acid (H₂pzdc). In situ oxalate formation as observed in this system has been been investigated using ¹H and ¹³C nuclear magnetic resonance spectroscopy, and a pathway for C₂O₄^{2鈥?/sup> anion formation under hydrothermal conditions has been elucidated. The oxalate ligands found in Nd₂(C₆H₂N₂O₄)₂(C₂O₄)(H₂O)₂ result from the oxidation of H₂pzdc, 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鈥揘 bond of the pyrazine ring, followed by hydrolysis/oxidation of the resulting species.}