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FeSA@CoNP Single-Atom Nanozyme with Tandem H2O2 Production and Activation for Organic Dye Degradation without External Oxidants
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DOI：10.1021/acsestengg.6c00252.png)
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Abstract
En 中文
Single-atom nanozymes (SANs) provide a sustainable alternative to conventional advanced oxidation processes (AOPs) by directly generating reactive oxygen species (ROS) from dissolved oxygen, thereby eliminating the need for external oxidizing agents, which pose a threat of secondary pollution problems and further complex post-treatment. Herein, we report a dual-active-site nanozyme catalyst that comprises atomically dispersed Fe single atoms (FeSA) and cobalt nanoparticles (CoNP) confined within nitrogen-doped carbon nanotubes, denoted as FeSA@CoNP. The prepared catalyst exhibits outstanding oxidase-like activity, efficiently oxidizing 3,3′,5,5′-Tetramethylbenzidine (TMB). Mechanistic studies reveal a synergistic pathway in which CoNP activates dissolved O2 to generate H2O2 in situ, which is subsequently converted on adjacent FeSA sites into multiple highly energetic ROS of •OH, O2•–, and 1O2. Kinetic study of oxidase enzymatic activity yields a Vmax = 1.94 × 10–7 M s–1, Km = 0.29 mM, and SA = 3.79 U/mg. In environmental applications, FeSA@CoNP achieves rapid Rhodamine B (RhB) degradation with a rate constant of 0.377 min–1 and complete pollutant removal without external oxidant addition. Compared with previously reported SANs, this work demonstrates a highly efficient, oxidant-free SAN platform with a promising potential for sustainable wastewater treatment.
Keywords:
Catalysts
Degradation
Free radicals
Oxidation
single-atom nanozyme
sustainability
oxidase-like activity
environmental health
pollutants degradation
In situ H2O2 production
synergetic reaction
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