Synthesis and applications of bimetallic metal-organic frameworks catalyst for activating peroxymonosulfate for carbamazepine degradation.

In this research, a series of bimetallic CuxZny-MOFs catalysts was constructed via a convenient solvothermal synthesis procedure by using the 2,3,6,7,10,11-hexaiminotriphenylene (HATP) ligand with copper and zinc metal ions. Among the series catalysts, Cu2Zn1-MOFs exhibited outstanding adsorption efficiency and degradation performance, and achieved 97.83% carbamazepine (CBZ) removal within 15 min using a catalyst dosage of 0.05 g L-1 and 0.5 mM peroxymonosulfate (PMS) concentration. The catalytic degradation rate constant of CBZ by Cu2Zn1-MOFs catalyst reached to 0.1833 min-1, which is 3.1 times higher than Cu-MOFs. In order to investigate the catalytic mechanism, density functional theory (DFT) calculations and experimental results were conducted which revealed the enhanced adsorption efficiency due to the incorporation of zinc into Cu-MOFs, thereby promoting the generation of reactive oxygen species in PMS activation. Furthermore, the CBZ degradation pathway was elucidated by detected the intermediates using LC/MS during the oxidation process. These findings highlighted the synergistic effects of bimetallic MOFs as highly efficient heterogeneous Fenton-like catalyst, which could expand the potential actual application.