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Spin-Regulated Fenton-Like Catalysis for Nonradical Oxidation over Metal Oxide@Carbon Composites

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dc.contributor.authorLi, B.
dc.contributor.authorLiu, Y.
dc.contributor.authorHu, K.
dc.contributor.authorDai, Q.
dc.contributor.authorChen, C.
dc.contributor.authorDuan, X.
dc.contributor.authorWang, S.
dc.contributor.authorWang, Y.
dc.date.issued2024
dc.descriptionPublished online: April 24, 2024
dc.description.abstractThe spin state of the transition metal species (TMs) has been recognized as a critical descriptor in Fenton-like catalysis. The raised spin state of dispersed TMs in carbon will enhance the redox processes with adsorbed peroxides and improve the oxidation performance. Nevertheless, establishing the spin-activity correlations for the encapsulated TM nanoparticles remains challenging because of the difficulties in fine-tuning the spin state of TM species and the insufficient understanding of orbital hybridization states upon interaction with peroxides. Here, the advantage of the fast-temperature heating/quenching of microwave thermal shock is taken to engineer the structure and spin state of encapsulated TMs within the N-doped graphitic carbons. The reduced TMs particle size and enhanced TMs-carbon coupling increase surface entropy and regulate eg electron filling of the high-spin TM-N coordination, endowing electrons with high mobility and facilitating peroxymonosulfate (PMS) adsorption. The strong interactions further uplift the PMS O 2p band position toward the Fermi level and thus elevate the oxidation potential of surface-activated PMS (PMS*) as the dominant nonradical species for pollutant degradation. The deciphered orbital hybridizations of engineered high-spin TM and PMS enlighten the smart design of spin-regulated nanocomposites for advanced water purification.
dc.description.statementofresponsibilityBofeng Li, Ya Liu, Kunsheng Hu, Qin Dai, Chunmao Chen, Xiaoguang Duan, Shaobin Wang, and Yuxian Wang
dc.identifier.citationAdvanced Functional Materials, 2024; 34(36):2401397-1-2401397-12
dc.identifier.doi10.1002/adfm.202401397
dc.identifier.issn1616-301X
dc.identifier.issn1616-3028
dc.identifier.orcidLiu, Y. [0000-0001-6329-5414]
dc.identifier.orcidHu, K. [0000-0002-8598-6336]
dc.identifier.orcidDuan, X. [0000-0001-9635-5807]
dc.identifier.orcidWang, S. [0000-0002-1751-9162]
dc.identifier.urihttps://hdl.handle.net/2440/142930
dc.language.isoen
dc.publisherWiley-VCH GmbH
dc.relation.grant22278436
dc.rights© 2024 Wiley-VCH GmbH
dc.source.urihttps://doi.org/10.1002/adfm.202401397
dc.subjectCo₃O₄; microwave-assisted synthesis; nonradical oxidation; peroxymonosulfate; spin state control
dc.titleSpin-Regulated Fenton-Like Catalysis for Nonradical Oxidation over Metal Oxide@Carbon Composites
dc.typeJournal article
pubs.publication-statusPublished

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