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Seven new ionic solids built on polyoxometalate (POM) anions and [Co(en)3] cations namely, [Co(en)3Mo8O26(H3O)(Cl)] (DMF)4 (H2O) (Co-Mo8-DMF), [α-PW12O40] [Co(en)3]∙6DMF (Co-W12P-DMF), [α-PW12O40] [Co(en)3]∙6DEF (Co-W12P-DEF), [α-PMo12O40][Co(en )3]∙5.5DMF (Co-Mo12P-DMF), [α-PMo12O40] [Co(en)3]∙6DEF (CoMo12P-DEF), [α-SiW12O40] [Co(en)3]3/2 [Cl]1/2∙6DMF∙3H2O (Co-W12SiDMF) and [α-SiW12O40][Co(en)3] ∙6DEF (Co-W12Si-DEF) have been synthesized from non aqueous (DMF/DEF) media and characterized by single-crystal X-ray diffraction. We attempt to understand if [Co(en)3] cations used in these reaction systems play a crucial role in controlling the assembly of these crystals. These ionic solids, after removal of the DMF or DEF molecules, are found to exhibit size selective H2 adsorption properties over N2. The amount of hydrogen adsorption was influenced by POM anion types and their orientations. CoMo12P-DEF has the highest (0.9 wt%) H2 uptake and CoW12P-DEF has the lowest (0.4 wt%) uptake among the series when the adsorbate pressure approached 1 atm. We believe that the successful synthesis of these seven new ionic solids and the discovery of their selective H2 adsorption properties, as a result of the cooperative behavior between their cationic/anionic component species, will open up new vistas in the search for polyoxometalate based materials with useful absorptive properties. We are further engaged in designing porous ionic crystals with functionalized interiors for enhanced gas adsorption capacity and higher selectivity.

Structure and selective gas adsorption study on POM-based ionic salts