An aliovalent mixed-metal framework DUT-174 [LiAl(2-methylimidazolate)(4)](n), isostructural to ZIF-8, was synthesized from lithium aluminum hydride (LiAlH4) and 2-methylimidazole (2-mImH) through dehydrogenation. Lithium and aluminum cations acting as alternating framework nodes are coordinated tetrahedrally by (2-mIm)(-). DUT-174 has a high specific surface area of 1149 m(2) g(-1) and CO2 uptake of 11.57 mmol g(-1) at 195 K.