A　Zn-II-based　metal-organic　framework　(MOF),　[Zn-2(bdpCHO)(2)]center　dot(DMF)(CH3CN)(H2O)(2)　(BUT-31)　is　reported　that　was　synthesized　by　the　reaction　between　a　newly　designed　aldehyde-tagged　polypyrazole　ligand　2,5-di(1H-pyrazol-4-yl)　benzaldehyde　(H(2)bdp-CHO)　and　a　zinc　salt.　BUT-31　has　a　unique　pillared　layered　framework　structure　with　3D　intersecting　channels　approximately　3.4-5.4　angstrom　in　size.　Powder　X-ray　diffraction　and　N-2　adsorption　experiments　revealed　that　BUT-31　is　rigid　and　permanently　porous　with　the　Brunauer-Emmett-Teller　surface　area　of　926　m(2)g(-1).　Notably,　this　MOF　tolerates　boiling　water　and　even　highly　basic　aqueous　solution　(4M　sodium　hydroxide),　although　dilute　acid　gradually　decomposes　its　framework.　Owing　the　permanent　porosity　and　chemical　stability　of　BUT31,　covalent　post-modification　of　the　free　aldehyde　group　exposed　on　the　pore　surface　was　accomplished　by　treating　the　MOF　in　a　concentrated　ammonia　solution　(25%)　at　near　room　temperature,　giving　rise　to　an　imine-functionalized　analogue　of　BUT-31.　Gas　adsorption　results　show　that　the　aldehyde-and　imine-functionalized　MOFs　have　high　CO2　adsorption　capacities,　as　well　as　CO2/N-2　and　CO2/CH4　adsorption　selectivities.