Metal- and Site-Specific Roles of High-Entropy Spinel Oxides in Catalytic Oxidative Polymerization of Water Contaminants

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dc.contributor.authorMo, Y.
dc.contributor.authorTian, Z.
dc.contributor.authorHu, K.
dc.contributor.authorRen, W.
dc.contributor.authorLu, X.
dc.contributor.authorDuan, X.
dc.contributor.authorWang, S.
dc.date.issued2025
dc.description.abstractHigh-entropy spinel oxides (HESOs) have emerged as promising catalysts due to their multimetal interactions, compositional flexibility, and superior structural stability; however, the roles of each metal in catalytic reactions remain elusive. In addition, catalytic organic recycling via polymerization has attracted increasing attention as a sustainable strategy for wastewater treatment. Herein, we synthesized HESOs incorporating five transition metals (Fe, Co, Ni, Cr, and Mn) using a low-temperature microwave-assisted method to achieve highly dispersed metal species in nanoparticles for catalytic peroxymonosulfate (PMS) activation for organic transformation and elucidate the different metal site catalysis. Comprehensive characterizations confirmed the single-phase spinel structure, high configurational entropy, and site-selective cation distribution among the tetrahedral and octahedral sites within the HESOs. The HESOs demonstrated superior activity in PMS activation for the polymerization of bisphenol A (BPA), outperforming single metal-based oxides. Mechanistic studies revealed that BPA degradation followed a nonradical electron transfer pathway mediated by surface catalyst-PMS* complexes. The enhanced catalytic activity was attributed to the distinct roles of individual metal components at different sites: Co served as the predominant electron donor, Cr facilitated strong PMS adsorption, and Ni supported the redox cycling of Co²⁺/Co³⁺. These metal-specific contributions synergistically enhanced the PMS activation efficiency, enabling BPA removal via oxidative polymerization with minimal oxidant consumption. Overall, this work provides in-depth insights into the metal- and site-specific roles in multisite synergy of HESOs and demonstrates their innovative application in Fenton-like catalysis toward fast water decontamination in a more selective and low-chemical-consumption manner for carbon recycling.
dc.description.statementofresponsibilityYalan Mo, Zhihao Tian, Kunsheng Hu, Wei Ren, Xiao Lu, Xiaoguang Duan, Shaobin Wang
dc.identifier.citationACS Catalysis, 2025; 15(8):5928-5942
dc.identifier.doi10.1021/acscatal.5c00854
dc.identifier.issn2155-5435
dc.identifier.issn2155-5435
dc.identifier.orcidMo, Y. [0000-0002-3267-3926]
dc.identifier.orcidHu, K. [0000-0002-8598-6336]
dc.identifier.orcidRen, W. [0000-0002-1299-0393]
dc.identifier.orcidLu, X. [0000-0002-8053-6897]
dc.identifier.orcidDuan, X. [0000-0001-9635-5807]
dc.identifier.orcidWang, S. [0000-0002-1751-9162]
dc.identifier.urihttps://hdl.handle.net/2440/146293
dc.language.isoen
dc.publisherAmerican Chemical Society
dc.relation.granthttp://purl.org/au-research/grants/arc/DP230102406
dc.relation.granthttp://purl.org/au-research/grants/arc/FL230100178
dc.rights©2025 American Chemical Society
dc.source.urihttps://doi.org/10.1021/acscatal.5c00854
dc.subjecthigh-entropy spinel oxides; site-selective cation distribution; metal-specific roles; multisite synergy; oxidative polymerization
dc.titleMetal- and Site-Specific Roles of High-Entropy Spinel Oxides in Catalytic Oxidative Polymerization of Water Contaminants
dc.typeJournal article
pubs.publication-statusPublished

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