期刊
NATURE
卷 549, 期 7670, 页码 78-+出版社
NATURE RESEARCH
DOI: 10.1038/nature23662
关键词
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资金
- NSAF [U1530101]
- National Natural Science Foundation of China [51374131]
Singly or doubly bonded polynitrogen compounds can decompose to dinitrogen (N-2) with an extremely large energy release. This makes them attractive as potential explosives or propellants(1-3), but also challenging to produce in a stable form. Polynitrogen materials containing nitrogen as the only element exist in the form of high-pressure polymeric phases(4-6), but under ambient conditions even metastability is realized only in the presence of other elements that provide stabilization. An early example is the molecule phenylpentazole, with a five-membered all-nitrogen ring, which was first reported in the 1900s(7) and characterized in the 1950s(8,9). Salts containing the azide anion (N-3(-))(10-12) or pentazenium cation (N-5(+))(13) are also known, with compounds containing the pentazole anion, cyclo-N-5(-), a more recent addition(14-16). Very recently, a bulk material containing this species was reported(17) and then used to prepare the first example of a solid-state metal-N-5 complex(18). Here we report the synthesis and characterization of five metal pentazolate hydrate complexes [Na(H2O)(N-5)]center dot 2H(2)O, [M(H2O)(4)(N-5)(2)]center dot 4H(2)O (M = Mn, Fe and Co) and [Mg(H2O)(6)(N-5)(2)]center dot 4H(2)O that, with the exception of the Co complex, exhibit good thermal stability with onset decomposition temperatures greater than 100 degrees C. For this series we find that the N-5(-) ion can coordinate to the metal cation through either ionic or covalent interactions, and is stabilized through hydrogen-bonding interactions with water. Given their energetic properties and stability, pentazole-metal complexes might potentially serve as a new class of high-energy density materials(19) or enable the development of such materials containing only nitrogen(20-23). We also anticipate that the adaptability of the N-5(-) ion in terms of its bonding interactions will enable the exploration of inorganic nitrogen analogues of metallocenes(24) and other unusual polynitrogen complexes.
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