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We clarified that the metal-centering octahedral pentazolate framework was entrapped by dual ionic-covalent bonds. More importantly, the covalent bonding can effectively enhance the chemical insensitivity and thermal stability, further preventing the autodecomposition of monatomic solid N5- anions into dinitrogen. Meanwhile, a unique topological pseudogap that attached to a metastable phase of ZnN4 salt is exposed for the first time, due to the dual effects of strong covalent sp2 hybridization interaction and the origin of ionic states.
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