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Type: | Journal article |
Title: | Redox-Active Polymers as Robust Electron-Shuttle Co-Catalysts for Fast Fe³⁺/Fe²⁺ Circulation and Green Fenton Oxidation |
Other Titles: | Redox-Active Polymers as Robust Electron-Shuttle Co-Catalysts for Fast Fe3+/Fe2+ Circulation and Green Fenton Oxidation |
Author: | Zhou, H. Peng, J. Duan, X. Yin, H. Huang, B. Zhou, C. Zhong, S. Zhang, H. Zhou, P. Xiong, Z. Ao, Z. Wang, S. Yao, G. Lai, B. |
Citation: | Environmental Science and Technology (Washington), 2023; 57(8):3334-3344 |
Publisher: | American Chemical Society |
Issue Date: | 2023 |
ISSN: | 0013-936X 1520-5851 |
Statement of Responsibility: | Hongyu Zhou, Jiali Peng, Xiaoguang Duan, Haoxiang Yin, Bingkun Huang, Chenying Zhou, Shuang Zhong, Heng Zhang, Peng Zhou, Zhaokun Xiong, Zhimin Ao, Shaobin Wang, Gang Yao, and Bo Lai |
Abstract: | Accelerating the rate-limiting Fe3+/Fe2+ circulation in Fenton reactions through the addition of reducing agents (or co-catalysts) stands out as one of the most promising technologies for rapid water decontamination. However, conventional reducing agents such as hydroxylamine and metal sulfides are greatly restricted by three intractable challenges: (1) self-quenching effects, (2) heavy metal dissolution, and (3) irreversible capacity decline. To this end, we, for the first time, introduced redox-active polymers as electron shuttles to expedite the Fe3+/Fe2+ cycle and promote H2O2 activation. The reduction of Fe3+ mainly took place at active N-H or O-H bonds through a proton-coupled electron transfer process. As electron carriers, H atoms at the solid phase could effectively inhibit radical quenching, avoid metal dissolution, and maintain long-term reducing capacity via facile regeneration. Experimental and density functional theory (DFT) calculation results indicated that the activity of different polymers shows a volcano curve trend as a function of the energy barrier, highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) gap, and vertical ionization potential. Thanks to the appropriate redox ability, polyaniline outperforms other redox-active polymers (e.g., poypyrrole, hydroquinone resin, poly(2,6-diaminopyridine), and hexaazatrinaphthalene framework) with a highest iron reduction capacity up to 5.5 mmol/g, which corresponds to the state transformation from leucoemeraldine to emeraldine. Moreover, the proposed system exhibited high pollutant removal efficiency in a flow-through reactor for 8000 bed volumes without an obvious decline in performance. Overall, this work established a green and sustainable oxidation system, which offers great potential for practical organic wastewater remediation. |
Keywords: | Fenton reactions redox-active polymers Fe3+/Fe2+ circulation electron shuttles sustainable chemistry |
Description: | Published: February 3, 2023 |
Rights: | © 2023 American Chemical Society |
DOI: | 10.1021/acs.est.2c07447 |
Grant ID: | http://purl.org/au-research/grants/arc/DE210100253 |
Published version: | http://dx.doi.org/10.1021/acs.est.2c07447 |
Appears in Collections: | Chemical Engineering publications |
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