The design and construction of "thermodynamically stable" metal-organic frameworks (MOFs) that can survive in liquid water,b oiling water,a nd acidic/basic solutions over aw ide pH range is highly desirable for many practicala pplications, especially adsorption-based gas separationsw ith obviouss calablep reparations. Herein,anew thermodynamically stable Ni MOF,{ [Ni(L)(1,4-NDC)(H 2 O) 2 ]} n (IITKGP-20;L= 4,4'-azobispyridine;1 ,4-NDC = 1,4-naphthalene dicarboxylic acid;I ITKGP stands for the Indian Institute of Technology Kharagpur), hasb een designed that displays moderate porosity with aB ET surfacea rea of 218 m 2 g À1 and micropores along the [10À1] direction. As an alternative to ac ost-intensive, cryogenic,h igh-pressure distillation process for the separation of hydrocarbons, MOFsh ave recently shown promise for such separations. Thus, towards an application standpoint, this MOF exhibits ah igher uptake of C 2 hydrocarbons over that of C 1 hydrocarbon under ambient conditions, with one of the highest selectivities basedo nt he ideal adsorbed solution theory (IAST)m ethod. Ac ombination of two strategies (the presence of stronger metal-N coordinationo ft he spacera nd the hydrophobicity of the aromatic moiety of the organic ligand) possibly makes the framework highly robust, even stable in boiling water and over aw ide range of pH 2-10, andr epresents the first example of at hermodynamically stableM OF displayinga2D structural network. Moreover, this material is easily scalable by heatingt he reaction mixture at reflux overnight. Because such separations are performedi nt he presence of water vapor and acidic gases, there is ag reat need to explore thermodynamically stable MOFs that retain not only structurali ntegrity,b ut also the porosityo ft he frameworks.