151. Electron cycling mechanism in Fe/Mn DSAzyme accelerates BPA degradation and nanoenzyme regeneration.
- Author
-
Lv X, Shu A, Shu L, Liu H, Liu Y, Cui K, Tang Y, and Chen X
- Subjects
- Nanotubes, Carbon chemistry, Electrons, Catalysis, Wastewater chemistry, Peroxidase chemistry, Peroxidase metabolism, Water Purification methods, Benzhydryl Compounds chemistry, Iron chemistry, Phenols chemistry, Hydrogen Peroxide chemistry, Manganese chemistry, Water Pollutants, Chemical chemistry
- Abstract
Peroxidase-like (POD-like) as a kind of new Fenton-like catalyst can effectively activate H
2 O2 to degrade organic pollutants in water, but improving the catalytic activity and stability of POD-like remains a challenging task. Here, we synthesized a novel dual single-atom nanoenzyme (DSAzyme) FeMn/N-CNTs with Fe-N4 and Mn-N4 bimetallic single-atom active centers by mimicking the active centers of natural enzymes and taking advantage of the synergistic effect between the dual metals. FeMn/N-CNTs DSAzyme showed significantly enhanced POD-like activity compared to monometallic-loaded Fe/N-CNTs and Mn/N-CNTs. Within the FeMn/N-CNTs/H2 O2 system, bisphenol A (BPA) could be removed 100 % within 20 min. DFT calculations show that Mn-N4 in FeMn/N-CNTs can readily adsorb negatively charged BPA molecules and capture electrons. Meanwhile, Fe-N4 sites can easily adsorb H2 O2 molecules, leading to their activation and splitting into strongly oxidizing hydroxyl radicals (·OH). Throughout this process, electrons are continuously recycled in BPA → Mn-N4 → Fe-N4 → H2 O2 , effectively promoting the regeneration of Fe2+ . Practical studies on wastewater and cycling experiments have demonstrated the great potential of this method for remediating water environments., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)- Published
- 2024
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