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In-situ green assembly of spherical Mn-based metal-organic composites by ion exchange for efficient electrochemical oxidation of organic pollutant.

In this study, we develop a facile ion exchange strategy for in-situ assembly of novel spherical metal-organic composites on a large scale. The functional groups (-NH2 , -COOH and -SO3 H) on chelating and exchange resins had significant effects on improving uniform distribution of metallic sites and metal-support interaction. Without any addition of H2 O2 , Mn-based metal-organic composites realized the recovery of waste metallic ions and exhibited high activity for methylene blue (MB) electro-Fenton degradation (97.8% decoloration and 54.7% TOC removal) within 150 min under low current density (7.53 mA·cm-2 ) and 3.0 g·L-1 catalyst dosage. Analyses of performance on different active sites (FeII , MnII , CoII , CeIII and CuII ) and supports clearly indicated that synergetic effect of MnII and organic supports played crucial roles in electrochemical oxidation. Kinetic rate constant of 0.037 min-1 and turn over frequency of 0.23 h-1 were much better than those of inorganic supported catalysts, which were attributed to intramolecular electron transfer greatly accelerating MnII /MnIII autocatalytic cycle. Meanwhile, possible degradation pathway of MB was proposed by analysis of oxidative intermediate products. Benefiting from excellent properties and millimeter-level size structure, metal-organic composites can be applied in wide pH range of 2.0-9.0 and easily separated in the industrial application.

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