The Nature of Molecular Hybridizations in Nanodiamonds for Boosted Fe(III)/Fe(II) Circulation
Date
2024
Authors
Hu, K.
Zhou, P.
Yang, Y.
Zhong, S.
Duan, X.
Wang, S.
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Journal article
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Environmental Science and Technology, 2024; 58(46):20665-20675
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Kunsheng Hu, Peng Zhou, Yangyang Yang, Shuang Zhong, Xiaoguang Duan, Shaobin Wang
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Abstract
Reducing agents have been frequently utilized as electron donors for Fe(II) generation to resolve the sluggish Fe(III) reduction in Fenton-like reactions, while their irreversible consumption necessitates a robust catalytic system that utilizes green electron donors such as H2O2. In this study, we used annealed nanodiamonds (NDs) as a collection of model catalysts with different sp2/sp3 ratios to investigate the roles of the molecular structure in boosting the Fenton-like reactions. The annealed NDs acted as an electron mediator to transfer electrons from H2O2 to surface-adsorbed Fe(III) for Fe(II) generation as well as an electron donor for direct Fe(III) reduction, driving Fe(II)-catalyzed H2O2 decomposition to produce massive hydroxyl radicals, demonstrating potential in the real-water matrixes. Galvanic cell experiments show that the contribution ratio of mediation and electron donation is 2.75:1, indicating that the majority of Fe(II) was generated through electron transfer from H2O2. Additionally, different carbon configurations (sp-sp2-sp3 hybridizations) were compared to assess the molecular structure-performance relationships in Fe(III) reduction. This study unveils the distinct functions of carbon molecular structures in driving Fe(III)/Fe(II) circulation and provides insights into sustainable Fenton oxidation driven by metal-free catalysis.
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© 2024 American Chemical Society