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Redox-Active Polymers as Robust Electron-Shuttle Co-Catalysts for Fast Fe³⁺/Fe²⁺ Circulation and Green Fenton Oxidation

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dc.contributor.authorZhou, H.
dc.contributor.authorPeng, J.
dc.contributor.authorDuan, X.
dc.contributor.authorYin, H.
dc.contributor.authorHuang, B.
dc.contributor.authorZhou, C.
dc.contributor.authorZhong, S.
dc.contributor.authorZhang, H.
dc.contributor.authorZhou, P.
dc.contributor.authorXiong, Z.
dc.contributor.authorAo, Z.
dc.contributor.authorWang, S.
dc.contributor.authorYao, G.
dc.contributor.authorLai, B.
dc.date.issued2023
dc.descriptionPublished: February 3, 2023
dc.description.abstractAccelerating 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.
dc.description.statementofresponsibilityHongyu 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
dc.identifier.citationEnvironmental Science and Technology, 2023; 57(8):3334-3344
dc.identifier.doi10.1021/acs.est.2c07447
dc.identifier.issn0013-936X
dc.identifier.issn1520-5851
dc.identifier.orcidZhou, H. [0000-0003-1117-1422]
dc.identifier.orcidDuan, X. [0000-0001-9635-5807]
dc.identifier.orcidZhong, S. [0000-0001-6103-5125]
dc.identifier.orcidWang, S. [0000-0002-1751-9162]
dc.identifier.urihttps://hdl.handle.net/2440/137565
dc.language.isoen
dc.publisherAmerican Chemical Society
dc.relation.granthttp://purl.org/au-research/grants/arc/DE210100253
dc.rights© 2023 American Chemical Society
dc.source.urihttps://doi.org/10.1021/acs.est.2c07447
dc.subjectFenton reactions
dc.subjectredox-active polymers
dc.subjectFe3+/Fe2+ circulation
dc.subjectelectron shuttles
dc.subjectsustainable chemistry
dc.subject.meshHydrogen Peroxide
dc.subject.meshIron
dc.subject.meshReducing Agents
dc.subject.meshOxidation-Reduction
dc.subject.meshElectrons
dc.titleRedox-Active Polymers as Robust Electron-Shuttle Co-Catalysts for Fast Fe³⁺/Fe²⁺ Circulation and Green Fenton Oxidation
dc.title.alternativeRedox-Active Polymers as Robust Electron-Shuttle Co-Catalysts for Fast Fe3+/Fe2+ Circulation and Green Fenton Oxidation
dc.typeJournal article
pubs.publication-statusPublished

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