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1.
ACS Environ Au ; 4(2): 56-68, 2024 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-38525020

RESUMO

Effective techniques for eliminating antibiotics from water environments are in high demand. The peracetic acid (PAA)-based advanced oxidation process has recently drawn increasing attention for its effective antibiotic degrading capability. However, current applications of PAA-based techniques are limited and tend to have unsatisfactory performance. An additional catalyst for PAA activation could provide a promising solution to improve the performance of PAA. Bulky metal-organic framework gels (MOGs) stand out as ideal catalysts for PAA activation owing to their multiple advantages, including large surface areas, high porosity, and hierarchical pore systems. Herein, a bimetallic hierarchical porous structure, i.e., FeMn13BTC, was synthesized through a facile one-pot synthesis method and employed for PAA activation in ofloxacin (OFX) degradation. The optimized FeMn MOG/PAA system exhibited efficient catalytic performance, characterized by 81.85% OFX degradation achieved within 1 h owing to the specific hierarchical structure and synergistic effect between Fe and Mn ions, which greatly exceeded the performance of the only PAA-catalyzed system. Furthermore, the FeMn MOG/PAA system maintained >80% OFX degradation in natural water. Quenching experiments, electron spin resonance spectra, and model molecular degradation revealed that the primary reactive oxygen species responsible for the catalytic effect was R-O•, especially CH3C(=O)OO•, with minor contributions of •OH and 1O2. Overall, introduction of the MOG catalyst strategy for PAA activation achieved high antibiotic degradation performance, establishing a paradigm for the design of heterogeneous hierarchical systems to broaden the scope of catalyzed water treatment applications.

2.
ACS Appl Mater Interfaces ; 13(10): 12463-12471, 2021 Mar 17.
Artigo em Inglês | MEDLINE | ID: mdl-33657796

RESUMO

Hollow core-shell catalytic nanoreactors have received tremendous attention due to their high mass transfer in catalysis applications. Herein, we present a novel type of well-arranged, hollow core-shell nanoreactors featured with a bimetallic porous Zn/Ni-MOF-2 shell and a tiny Au nanoparticle core. The well-designed hollow Au@Zn/Ni-MOF-2 nanoreactors were constructed through the strategy of a facile one step from a rare crystal-structure transformation without any additional template. These nanoreactors exhibit outstanding multifunctional catalysis for a broad range of alcohol oxidation under the green oxidant environment. Moreover, such hollow nanoreactors show excellent recyclability toward the selective alcohol oxidation. These findings might provide a promising platform for a general construct of various metal-organic framework-based hollow core-shell nanostructures and further highly augmented catalytic applications.

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