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Two new organic-inorganic compounds [(CH2)5NH2]3[PMo12O40]·3[(CH2)5NH] 1 and [(CH2)5NH2]6[P2Mo18O62]·5H2O 2 have been synthesized using conventional and hydrothermal methods, respectively, and characterized by elemental analyses, IR, TG and single-crystal X-ray diffraction. X-ray analyses show that in these compounds heteropolymolybdates [PMo12O40]3- and [P2Mo18O62]6- are reserved their Keggin or Dawson structures and linked to piperidine through electrostatic and hydrogen-bonding interactions.