Abstract
The efficient discrimination of industrially relevant gases, particularly those with closely analogous physicochemical properties, remains a formidable challenge within the realm of adsorptive separation technologies. Achieving satisfactory separation efficiency poses stringent requirements on the precise control over the pore structures of adsorbents. Here we introduce a strategy for the precise modulation of pore structures in a carbonate-pillared Zn-triazolate framework, Zn(2)(datrz)(2)CO(3) (datrz = 3,5-diamino-1,2,4-triazolate), through the straightforward adjustment of the solvothermal synthesis temperature. Utilizing this approach, we have successfully fabricated a series of Zn(2)(datrz)(2)CO(3) materials with tunable pore structures while maintaining the framework composition and overall connectivity. These materials demonstrate selective recognition for challenging gas mixtures, including C(3)H(6)/C(3)H(8), CO(2)/CH(4), and CO(2)/N(2). Density functional theory (DFT) calculations confirm that the precisely engineered pore environment plays a decisive role on selective gas adsorption. Further, the high reproducibility and scalability of this temperature-controlled synthesis method underscore its immense potential for industrial-scale applications in gas purification and separation processes.