In Situ Growth of Self-Assembled ZIF-8–Aminoclay Nanocomposites with Enhanced Surface Area and CO₂ Uptake

Self-assembly of metal–organic framework (MOF) nanoparticles (NPs) with a functional material can result in MOF nanocomposites having new and advanced properties along with the fabrication of new nanoscopic structures. However, such assembly of MOFs has not been realized to date. Here we report self-assembled nanocomposites of the zeolitic imidazolate framework (ZIF-8) and layered aminoclay (AC) for the first time, and the ZIF-8@AC composites exhibit significantly enhanced adsorption properties in comparison to those of pristine ZIF-8 nanoparticles. Four different composites denoted as <b>ZIF-8@AC-1</b>, <b>ZIF-8@AC-2</b>, <b>ZIF-8@AC-3</b>, and <b>ZIF-8@AC-4</b> were synthesized by varying the clay content, and their AC contents were found to be 12.1, 18.3, 22.2, and 27.2 wt %, respectively. The composites were thoroughly characterized by PXRD, FTIR, Raman, and various microscopic techniques (FESEM, TEM, and STEM). The formation of the composites is driven by the specific interaction between unsaturated Zn­(II) sites of ZIF-8 nanoparticles and NH₂ groups of the aminoclay, which was validated from ζ potential and Raman spectroscopic measurements. The adsorption studies of the desolvated composites were also carried out in detail. The best performance is achieved with one of the composites, which exhibits a 42% increase in BET surface area while CO₂ uptake at 298 K is doubled in comparison to the ZIF-8 nanoparticles.