Abstract:
Recently, the synthesis of metal-organic frameworks (MOFs) using recycled materials has become increasingly attractive to many researchers because it can be a strategy to support a circular economic system. In this work, Zn-based MOFs were synthesized utilizing zinc extracted from the electrode of spent alkaline batteries, along with the terephthalic acid (TPA) organic ligand derived from the acid hydrolysis of polyethylene terephthalate (PET) plastic waste. The investigation involved two different synthesis approaches, namely the one-pot synthesis and the two-step synthesis. The one-pot synthesis was performed by using the zinc acid-leached solution for depolymerizing PET and also for synthesizing MOF in one pot. The depolymerization reaction condition was first conducted at 130 °C for 6 h at the metal: ligand (M:L) mole ratio of 3:1. After 6h, the pH was adjusted at three different pH levels (not adjusted, 5, and 6) and continued heating for 12 h to synthesize the MOF. In the two-step synthesis, it involved adding the zinc leached solution after PET has been depolymerized at 130 °C for 12 hours. The solution was then adjusted to five different pH levels (not adjusted, 4, 6, 9, and 12) and continued heating for 12h to produce the MOF. All synthesized MOF Zn-TPA products were characterized using a Fourier-transform infrared spectrometer, powder X-ray diffraction, scanning electron microscopy, and a zeta potential analyzer, and were subsequently evaluated for their antibiotic adsorption applications. The synthetic antibiotic of the quinolone class, enrofloxacin (ENR), was employed to represent an accumulated antibiotic in the environment that can contribute to bacterial antibiotic resistance. In the adsorption study, various parameters such as adsorption kinetics, adsorption isotherms, the influence of pH, and interference of salts were investigated. The results revealed that the two-step synthesis products exhibited a higher adsorption capacity compared to the one-pot products. The MOF Zn-TPA exhibited efficient ENR absorption at pH 8 and 10 but decreased at pH 6. At pH 4 and 12, explicit adsorption was not observed. Among all MOF Zn-TPA products, the MOF Zn-TPA synthesized using the two-step method at pH 9 displayed characteristic MOF 69-c, demonstrating a high adsorption capacity across a wide pH range (6-10) and stability in moisture, making it an optimized Zn-TPA MOF. When tested for ENR adsorption in canal water, the two-step synthesized products maintained a high adsorption capacity, in contrast to the low capacity observed in simulated seawater due to the presence of high ion concentration. While our synthesized MOF was not able to regenerate, it can be reused for many cycles until its active sites are completely utilized.
Thammasat University. Thammasat University Library