دانلود رایگان مقاله تخریب شبه فنتون بیسفنول A کاتالیز شده با مزوپور Cu/TUD-1

Abstract

A family of copper oxide catalysts with loadings spanning 1–5 wt% were dispersed on a three dimensional, mesoporous TUD-1 silica through a hydrothermal, surfactant-free route employing tetraethylene glycol as a structure-directing agent. Their bulk and surface properties were characterized by N2 physisorption, XRD, DRUVS, EPR, TEM and Raman spectroscopy, confirming the expected mesoporous wormhole/foam support morphology and presence of well-dispersed CuO nanoparticles (∼5–20 nm). The catalytic performance of Cu/TUD-1 was evaluated as heterogeneous Fenton-like catalysts for Bisphenol A (BPA) oxidative degradation in the presence of H2O2 as a function of [H2O2], and CuO loading. Up to 90.4% of 100 ppm BPA removal was achieved over 2.5 wt% Cu/TUD-1 within 180 min, with negligible Cu leaching into the treated water.

4. Conclusion

A family of copper modified TUD-1 catalysts were synthesized with Cu loadings between 0.9–5.4 wt% employing TEG as a soft template. The resulting materials exhibited high surface areas and an amorphous, disordered mesopore network, containing isolated Cu2+ ions in a tetrahedral coordination (presumably within the silica framework) alongside CuO oligomers. High copper loadings favor the formation of CuO nanocrystallites dispersed across the TUD-1 support. Cu/TUD-1 is an excellent catalyst BPA oxidative degradation in the presence of H2O2, with the optimum 2.5 wt% Cu/TUD-1 achieving 90.4% BPA removal in 180 min. Spin trap EPR measurements confirm that oxidation occurs via the generation of •OH radicals from H2O2, especially over isolated/oligomeric Cu2+ species, through a Fenton-like mechanism. Excitation−emission matrix fluorescence spectroscopy revealed that oxidation was accompanied by a loss of aromaticity and molecular fragmentation, while kinetic analysis confirmed that BPA degradation was first order in the pollutant independent of copper loading. Cu/TUD-1 exhibited negligible deactivation over five recycles, within minimal Cu leaching (0.0027 mg/L).