Two mixed alkali-metal borates, KLi[BO]·0.5HO () and [(μ-OH)@(NaLi)][BO]·0.5B(OH) (), have been prepared under solvothermal conditions. Both of them are obtained in the same synthetic system and contain a BO cluster as the structural-building unit (SBU) but exhibit quite different structural features. is a centric three-dimensional (3D) oxoboron (B-O) framework, where templated mixed K and Li cations occupied the cavities of the structure. crystallizes in an acentric space group under the templating effect of a unique acentric alkali-metal cluster [(μ-OH)@(NaLi)]. The SBU of is also the BO cluster, which acts as six-connected nodes linked together to form a 3D B-O framework, showing different characters from because of two types of templates; the acentric [(μ-OH)@(NaLi)] clusters and the electroneutral B (OH) groups fill in two different cages in the framework and further connect each other via Na-O-B bonds to build a novel two-dimensional (2D) wavy bricklike network, resulting in a 3D B-O framework interpenetrated by a 2D [(μ-OH)@(NaLi)]-B(OH) network. As a crystal material with an acentric space group, shows a good second harmonic generation response of about 2.8 times that of KDP (KHPO) and has a cutoff edge below 190 nm, which suggests that is a potential deep-UV NLO material.
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