Nano Pd0 particle confined within the pores of UiO-66(Zr)-F4 for efficient destruction of carbamazepine by the hydrogen-accelerated catalytic Fenton reaction
摘要
Refractory wastewater treatment via Fenton reactions is hindered by iron sludge. Herein, fluorinated UiO-66(Zr)-F4 was employed as a hydrogen-storage carrier to confine Pd⁰ catalytic centers, and an [H]-mediated (H2-precursored) Fenton-like system was constructed for carbamazepine degradation under ambient conditions. With 25 μM Fe2 + and 60 mL min⁻1 H2 flow, 53% carbamazepine removal was achieved in 1 h via ⋅OH/1O2 oxidation, and > 59% efficiency was retained over six 3-h cycles. However, [H]-driven hydrogen spillover reduced C-F bonds, causing a 92.3% drop in specific surface area that compromised long-term stability. It was concluded that fluorination is suboptimal; modulating the carrier’s hydrophobicity via electron-donating groups (instead of fluorination) is critical for stable Zr-MOF-based catalysts in [H]-assisted advanced oxidation, offering alternative perspectives for process optimization.
Graphical abstract