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A novel heterogeneous co(Ⅱ)-fenton-like catalyst for efficient photodegradation by visible light over extended pH

Science China Chemistry 2020年第12期63卷 1825-1836页

作者： Wu-Hua Chen Jin-Hua Xiong Xue Teng Jin-Xiao Mi Zhi-Biao Hu Haifeng Wang Zuofeng Chen Fujian Provincial colleges and University Engineering Research Center of Solid Waste Resource Utilization(Longyan University) College of Chemistry and Material ScienceLongyan UniversityLongyan 364012China Shanghai Key Laboratory of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China Key Laboratory for Advanced Materials Centre for Computational Chemistry and Research Institute of Industrial CatalysisEast China University of Science and TechnologyShanghai 200237China Department of Materials Science and Engineering College of MaterialsXiamen UniversityXiamen 361005China

A novel co^Ⅱ-fenton-like heterogeneous catalyst,(H3O)2[co^Ⅱ(phen)(H2O)2]2[Mo^Ⅵ5O15(PO4)2]·4H2O (phen=1,10-phenanthroline,C12N2H8)(1),is synthesized and utilized for photocatalytic degradation of organic dyes and antibiotic in a wide range of *** experimental results show that 1 acting as the fenton-like catalyst with H2O2 exhibits remarkable activity at pH 3–9 under vis-light irradiation and is merited with excellent recyclability and reusability.A variety of analytical methods,including in-situ electron paramagnetic resonance (EPR) spectroscopy and density functional theory (DFT) calculations,are applied to study the mechanism on generation of·OH and O2^·-radicals for photocatalytic *** suggests that,unlike the classical fenton process involving the redox transformation of the central cations,the generation of·OH and O2^·-radicals is associated with the substitution of the coordinating water molecules at co(Ⅱ) by H2O2 and/or OOH^-,followed by the light-driven O–O bond cleavage and *** outcomes of this study are striking which overcome the obstacles in the classical Fe^Ⅱ-fenton process,including the slow redox transformation between Fe(Ⅱ) and Fe(Ⅲ) and the production of massive iron precipitates especially at elevated *** opens up new avenues for the development of the high-performance fenton(-like) catalysts for photocatalytic degradation over extended pH and provides new insight into the related process.

关键词： co^Ⅱ-fenton-like reagent polyoxometalate photocatalytic degradation density functional theory(DFT)calculations in-situ EPR spectroscopic analysis

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