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Chemosphere. 2019 Aug 31;239:124612. doi: 10.1016/j.chemosphere.2019.124612. [Epub ahead of print]

Enhanced mineralization of oxalate by highly active and Stable Ce(III)-Doped g-C3N4 catalyzed ozonation.

Author information

1
State Key Laboratory of Pollution Control and Resources Reuse, School of Environmental Science & Engineering, Tongji University, Shanghai, 200092, PR China; Shanghai Institute of Pollution Control Ecological Security, Shanghai, 200092, PR China.
2
Department of Civil Engineering, The University of Hong Kong, Pokfulam Road, Hong Kong, PR China.
3
State Key Laboratory of Pollution Control and Resources Reuse, School of Environmental Science & Engineering, Tongji University, Shanghai, 200092, PR China; Shanghai Institute of Pollution Control Ecological Security, Shanghai, 200092, PR China. Electronic address: wudeli@tongji.edu.cn.

Abstract

The degradation of carboxylic acid has been identified as one of the rate-determining steps in the mineralization of organic pollutants by ozonation. In this study, Ce(III)-doped graphitic carbon nitride (Ce-CN) composites with different Ce(III) contents were synthesized and used as catalysts for the ozonation of oxalate. The morphology and structure of the Ce-CN were comprehensively characterized using various techniques such as SEM, XRD, FTIR, and XPS. The results show that the structure of g-C3N4 provided an ideal site for the accommodation of Ce(III) and thus facilitated the formation of surface hydroxyl groups. With 2.5%Ce-CN as a catalyst, the degradation efficiency of oxalate was increased by 47.1% after reaction for 30 min. The decomposition of ozone was accelerated in the presence of Ce-CN. Hydroxyl radicals were recorded by electron spin resonance and identified as the major actives species. Under the catalysis of 2.5%Ce-CN, the production of hydroxyl radicals was increased by 40%. The Ce(III) and surface hydroxyl groups that distributed uniformly on the surface of Ce-CN were speculated as the dual catalytic sites for the complexation of oxalate and activation of ozone, respectively. Ce-CN had a high stability and reutilization capability. It is proposed that a complex was formed between surface Ce(III) and oxalate, and this complex could be more easily attacked by the surrounding ozone and hydroxyl radicals than free oxalate. As oxalate is a typical recalcitrant carboxylic acid, the findings from this study are expected to promote the application of ozonation in the removal of organic pollutants.

KEYWORDS:

Catalytic ozonation; Cerium; Graphitic carbon nitride; Mineralization; Surface hydroxyl groups

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