[LiNa(N_5)_2(H_2O)_4]·H_2O:一种含螺旋链的新型双金属五唑骨架（英文）
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摘要
过去一个世纪以来,探索合成含有五唑阴离子(cyclo-N_5~-)的聚氮化合物吸引了科学家们的极大兴趣.本论文报道了一例基于异质双金属的五唑骨架,[LiNa(N_5)_2(H_2O)_4]·H_2O(1),并对其结构和热性质进行了表征.单晶X射线衍射表明化合物1具有三维超分子结构,其中相邻的{Li(H_2O)_2(N_5)_5}三聚体之间通过O–H···N氢键作用形成左手型和右手型螺旋链结构.化合物1在室温条件下具有良好的热稳定性,五唑环在106.1°C开始分解.本研究对于探索五唑阴离子的配位化学以及相关聚氮材料提供了新思路.
引文
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2 Christe KO.Recent advances in the chemistry of N5+,N5-and high-oxygen compounds.Prop Explos Pyrotech,2007,32:194-204
3 Lu M.Opinion on the energy level of metal-free pentazolate salts.Chin J Energ Mater,2017,25:530-532
4 Christe KO,Wilson WW,Sheehy JA,et al.N5+:A novel homoleptic polynitrogen ion as a high energy density material.Angew Chem Int Ed,1999,38:2004-2009
5 Huisgen R,Ugi I.Zur L?sung eines klassischen Problems der organischen Stickstoff-Chemie.Angew Chem,1956,68:705-706
6 Zhang C,Sun C,Hu B,et al.Investigation on the stability of multisubstituted arylpentazoles and the influence on the generation of pentazolate anion.J Energetic Mater,2016,34:103-111
7 Carlqvist P,?stmark H,Brinck T.The stability of arylpentazoles.JPhys Chem A,2004,108:7463-7467
8 Geiger U,Elyashiv A,Fraenkel R,et al.The Raman spectrum of dimethylaminophenyl pentazole(DMAPP).Chem Phys Lett,2013,556:127-131
9 Vij A,Pavlovich JG,Wilson WW,et al.Experimental detection of the pentaazacyclopentadienide(pentazolate)anion,cyclo-N5-.Angew Chem Int Ed,2002,41:3051-3054
10 Butler RN,Stephens JC,Burke LA.First generation of pentazole(HN5,pentazolic acid),the final azole,and a zinc pentazolate salt in solution:A new N-dearylation of 1-(p-methoxyphenyl)pyrazoles,a2-(p-methoxyphenyl)tetrazole and application of the methodology to 1-(p-methoxyphenyl)pentazole.Chem Commun,2003,1016-101711 Bazanov B,Geiger U,Carmieli R,et al.Detection of cyclo-N5-in THF solution.Angew Chem,2016,128:13427-13429
12 Butler RN,Hanniffy JM,Stephens JC,et al.A ceric ammonium nitrate N-dearylation of N-p-anisylazoles applied to pyrazole,triazole,tetrazole,and pentazole rings:Release of parent azoles.generation of unstable pentazole,HN5/N5-,in solution.J Org Chem,2008,73:1354-1364
13 Bazanov B,Geiger U,Grinstein D,et al.N5-in solution:isotopic labeling and further details of its synthesis by phenyl pentazole reduction.J Phys Chem A,2017,121:6727-6731
14 Schroer T,Haiges R,Schneider S,et al.The race for the first generation of the pentazolate anion in solution is far from over.Chem Commun,2005,38:1607-1609
15 Zhang C,Sun C,Hu B,et al.Synthesis and characterization of the pentazolate anion cyclo-N5-in(N5)6(H3O)3(NH4)4Cl.Science,2017,355:374-376
16 Xu Y,Wang Q,Shen C,et al.A series of energetic metal pentazolate hydrates.Nature,2017,549:78-81
17 Xu Y,Wang P,Lin Q,et al.A carbon-free inorganic-metal complex consisting of an all-nitrogen pentazole anion,a Zn(II)cation and H2O.Dalton Trans,2017,46:14088-14093
18 Zhang C,Yang C,Hu B,et al.A symmetric Co(N5)2(H2O)4?4H2Ohigh-nitrogen compound formed by cobalt(II)cation trapping of a cyclo-N5-anion.Angew Chem Int Ed,2017,56:4512-4514
19 Xu Y,Lin Q,Wang P,et al.Syntheses,crystal structures and properties of a series of 3D metal-inorganic frameworks containing pentazolate anion.Chem Asian J,2018,13:1669-1673
20 Sun C,Zhang C,Jiang C,et al.Synthesis of AgN5and its extended3D energetic framework.Nat Commun,2018,9:1269
21 Xu Y,Lin Q,Wang P,et al.Stabilization of the pentazolate anion in three anhydrous and metal-free energetic salts.Chem Asian J,2018,13:924-928
22 Xu Y,Wang P,Lin Q,et al.Self-assembled energetic 3D metalorganic framework[Na8(N5)8(H2O)3]nbased on cyclo-N5-.Dalton Trans,2018,47:1398-1401
23 Christe KO.Polynitrogen chemistry enters the ring.Science,2017,355:351
24 Zhang W,Wang K,Li J,et al.Stabilization of the pentazolate anion in a zeolitic architecture with Na20N60and Na24N60nanocages.Angew Chem Int Ed,2018,57:2592-2595
25 Steele BA,Stavrou E,Crowhurst JC,et al.High-pressure synthesis of a pentazolate salt.Chem Mater,2017,29:735-741
26 Laniel D,Weck G,Gaiffe G,et al.High-pressure synthesized lithium pentazolate compound metastable under ambient conditions.J Phys Chem Lett,2018,9:1600-1604
27 Wang PC,Xu YG,Wang Q,et al.Self-assembled energetic coordination polymers based on multidentate pentazole cyclo-N5-.Sci China Mater,2018,doi:10.1007/s40843-018-9268-0