Hierarchical Porous Bimetallic FeMn Metal-Organic Framework Gel for Efficient Activation of Peracetic Acid in Antibiotic Degradation

Lu Zheng; Jiarui Fu; Baolv Hua; Yi-Nan Wu; Yifan Gu; Nianqiao Qin; Fengting Li

doi:10.1021/acsenvironau.3c00041

Hierarchical Porous Bimetallic FeMn Metal-Organic Framework Gel for Efficient Activation of Peracetic Acid in Antibiotic Degradation

ACS Environ Au. 2023 Dec 5;4(2):56-68. doi: 10.1021/acsenvironau.3c00041. eCollection 2024 Mar 20.

Authors

Lu Zheng^{1

2}, Jiarui Fu^{1

2}, Baolv Hua^{1

2}, Yi-Nan Wu^{1

2}, Yifan Gu^{1

2}, Nianqiao Qin^{1

2}, Fengting Li^{1

2}

Affiliations

¹ State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China.
² Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China.

Abstract

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.