Fabrication and catalytic performance of meso-ZSM-5 zeolite encapsulated ferric oxide nanoparticles for phenol hydroxylation

摘要

An encapsulation-structured Fe_(2)O_(3)@mesoZSM-5(Fe@MZ5)was fabricated by confining Fe_(2)O_(3) nanoparticles(ca.4 nm)within the ordered mesopores of hierarchical ZSM-5 zeolite(meso-ZSM-5),with ferric oleate and amphiphilic organosilane as the iron source and meso-porogen,respectively.For comparison,catalysts with Fe_(2)O_(3)(ca.12 nm)encapsulated in intra-crystal holes of meso-ZSM-5 and with MCM-41 or ZSM-5 phase as the shell were also prepared via sequential desilication and recrystallization at different pH values and temperatures.Catalytic phenol hydroxylation performance of the as-prepared catalysts using H_(2)O_(2) as oxidant was compared.Among the encapsulation-structured catalysts,Fe@MZ5 showed the highest phenol conversion and hydroquinone selectivity,which were enhanced by two times compared to the Fe-oxide impregnated ZSM-5(Fe/Z5).Moreover,the Fe-leaching amount of Fe@MZ5 was only 3% of that for Fe/Z5.The influence of reaction parameters,reusability,and ·OH scavenging ability of the catalysts were also investigated.Based on the above results,the structure-performance relationship of these new catalysts was preliminarily described.