Modeling the Kinetics of Contaminants Oxidation and the Generation of Manganese(III) in the Permanganate/Bisulfite Process

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State Key Laboratory of Pollution Control and Resources Reuse, Tongji University, Shanghai 20092, P. R. China
State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin, Heilongjiang 150090, P. R. China
§ School of Civil and Environmental Engineering, University of New South Wales, Sydney, New South Wales 2052, Australia
Key Laboratory of Yangtze River Water Environment, Ministry of Education, College of Environment Science and Engineering, Tongji University, Shanghai 200092, P. R. China
*E-mail: [email protected]; phone: +86-21-65980956; fax: +86-21-65986313.
Cite this: Environ. Sci. Technol. 2016, 50, 3, 1473–1482
Publication Date (Web):December 28, 2015
https://doi.org/10.1021/acs.est.5b05207
Copyright © 2015 American Chemical Society
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Abstract

Permanganate can be activated by bisulfite to generate soluble Mn(III) (noncomplexed with ligands other than H2O and OH) which oxidizes organic contaminants at extraordinarily high rates. However, the generation of Mn(III) in the permanganate/bisulfite (PM/BS) process and the reactivity of Mn(III) toward emerging contaminants have never been quantified. In this work, Mn(III) generated in the PM/BS process was shown to absorb at 230–290 nm for the first time and disproportionated more easily at higher pH, and thus, the utilization rate of Mn(III) for decomposing organic contaminant was low under alkaline conditions. A Mn(III) generation and utilization model was developed to get the second-order reaction rate parameters of benzene oxidation by soluble Mn(III), and then, benzene was chosen as the reference probe to build a competition kinetics method, which was employed to obtain the second-order rate constants of organic contaminants oxidation by soluble Mn(III). The results revealed that the second-order rate constants of aniline and bisphenol A oxidation by soluble Mn(III) were in the range of 105–106 M–1 s–1. With the presence of soluble Mn(III) at micromolar concentration, contaminants could be oxidized with the observed rates several orders of magnitude higher than those by common oxidation processes, implying the great potential application of the PM/BS process in water and wastewater treatment.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.5b05207.

  • The experimental procedure conducted in SFS, details of competition kinetics, relative rate method, evolution of UV–visible spectra at different wavelengths in the PM/BS process, reduction kinetics of permanganate by bisulfite in the absence and presence of benzene, degradation of BPA, the evolution of absorbance at 258 nm under different conditions, the generation kinetics of phenol during benzene oxidation, the correlation of utilization rates of Mn(III) with the amounts of phenol generated in the process of benzene oxidation and the amounts of BPA removed by the PM/BS process, the second-order rate constants of aniline and BPA oxidation by various oxidants, relative rate of BPA oxidation and phenol generation, the second-order rate constants of phenol generation, and the utilization rate of Mn(III). (PDF)

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