RESUMO
The establishment of reticular chemistry has significantly facilitated the development of porous materials, especially for metal-organic frameworks (MOFs). On the other hand, as an alternative approach, in situ "one-pot" strategy has been explored as a promising approach to constructing MOFs, in which the synthesis of organic linkers and the sequential construction of MOFs are integrated into one solvothermal condition. This strategy can efficiently avoid the limitations faced in the traditional construction method, such as time-consuming organic synthesis and multiple separation and purification. Herein, inspired by the reaction of aldehydes and o-phenylenediamine and deep structural analysis of UiO-68, a series of tetra-, hexa-, and octa-topic carboxylic acids are synthesized using 2',3'-diamino-[1,1':4',1'"-terphenyl]-4,4'"-dicarboxylic acid and di-, tri-, and tetra-topic aldehydes as precursor. Then nine multicarboxylate-based zirconium MOFs (Zr-MOFs) are successfully constructed via the combination of reticular chemistry and in situ "one-pot" strategy. The resultant Zr-MOFs can be regarded as the partial face decoration of UiO-68. More importantly, the emission properties of resultant Zr-MOFs can be well controlled using aldehydes with tunable electronic structures. This work provides a new path to rational design and construction of porous materials with specific structures guided by reticular chemistry and conducted using in situ "one-pot" strategy.
RESUMO
In the present work, we report a "two-in-one" strategy to construct single-linker-based pillar-layered metal-organic frameworks (PL-MOFs) guided by reticular chemistry via an in situ "one-pot" approach. Two carboxyl groups and one pyridine group are integrated into one molecular skeleton to form bifunctional organic linkers via the reaction of pyridine-containing aldehyde and bicarboxylate-containing o-phenylenediamine. During the synthesis of organic linkers, two zinc-based PL-MOFs, non-interpenetrated HIAM-3016-op and two-fold interpenetrated HIAM-3017-op, can be simultaneously constructed. The different interpenetrations for these two PL-MOFs can be attributed to the increased length of the pyridine-containing moiety. HIAM-3017-op can be utilized for Cr2O72- detection with excellent sensitivity and selectivity. The present work not only provides a novel insight to design and prepare PL-MOFs with specific structures guided by reticular chemistry, but also indicates the universality of the in situ "one-pot" strategy to construct porous materials.