Activation of Persulfates by Graphitized Nanodiamonds for Removal of Organic Compounds

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Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06511, United States
School of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), San 31, Hyoja-dong, Pohang 790-784, Republic of Korea
§ Future Environmental Research Center, Korea Institute of Toxicology (KIT), Jinju, 660-844, Republic of Korea
Human and Environmental Toxicology Program, University of Science and Technology (UST), Daejeon, 305-350, Republic of Korea
School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulju-gun, Ulsan 689-798, Republic of Korea
*(C.L.) Phone: +82-52-217-2812; fax: +82-52-217-2809; e-mail: [email protected]
*(J.-H.K.) Phone: +1-203-432-4386; fax: +1-203-432-4387; e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2016, 50, 18, 10134–10142
Publication Date (Web):September 2, 2016
https://doi.org/10.1021/acs.est.6b02079
Copyright © 2016 American Chemical Society
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Abstract

This study introduces graphited nanodiamond (G-ND) as an environmentally friendly, easy-to-regenerate, and cost-effective alternative catalyst to activate persulfate (i.e., peroxymonosulfate (PMS) and peroxydisulfate (PDS)) and oxidize organic compounds in water. The G-ND was found to be superior for persulfate activation to other benchmark carbon materials such as graphite, graphene, fullerene, and carbon nanotubes. The G-ND/persulfate showed selective reactivity toward phenolic compounds and some pharmaceuticals, and the degradation kinetics were not inhibited by the presence of oxidant scavengers and natural organic matter. These results indicate that radical intermediates such as sulfate radical anion and hydroxyl radical are not majorly responsible for this persulfate-driven oxidation of organic compounds. The findings from linear sweep voltammetry, thermogravimetric analysis, Fourier transform infrared spectroscopy, and electron paramagnetic resonance spectroscopy analyses suggest that the both persulfate and phenol effectively bind to G-ND surface and are likely to form charge transfer complex, in which G-ND plays a critical role in mediating facile electron transfer from phenol to persulfate.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.6b02079.

  • Detailed experimental setup and procedure information on GC/MS system for phenol oxidation products analysis (Text S1), water quality parameters of field water samples (Table S1), phenol removal by G-NDs/PDS system with and without phosphate buffer solution (Figure S1), phenol removal by G-NDs/PDS system with and without dissolved oxygen (Figure S2), photographs and XPS spectra of G-NDs prepared at different annealing temperatures (Figure S3), HR-TEM images of G-ND (Figure S4), particles size distribution and average particles size for aqueous suspension of G-ND measured by dynamic light scattering (Figure S5), phenol oxidation by surface modification nanodiamonds without persulfate systems (Figure S6), phenol removal and pseudo first order rate constant for the removal of phenol by G-NDs/PDS system as a function of G-NDs loading and phenol concentrations (Figure S7), decomposition of phenol and oxyanions by G-NDs in the presence of oxyanions (Figure S8), BET specific surface area of carbon-materials (Figure S9), FT-IR spectrum of G-NDs/PDS system with and without UV treatment (Figure S10), EPR spectra obtained by spin trapping with DMPO in the Fe(II)/H2O2 and G-NDs/PDS system at acidic pH and neutral pH (Figure S11), the GC/MS spectrum of intermediates for the removal of phenol by G-NDs/PDS system (Figure S12), removal and recovery of phenol by G-NDs with and without persulfate systems (Figure S13), phenol removal by G-NDs/PDS system with different type of tap water (Figure S14) (PDF)

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