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Activation of peroxymonosulfate by carbonaceous oxygen groups: experimental and density functional theory calculations

Paper ID Volume ID Publish Year Pages File Format Full-Text
44739 46344 2016 8 PDF Available
Title
Activation of peroxymonosulfate by carbonaceous oxygen groups: experimental and density functional theory calculations
Abstract

•The roles of oxygen functional groups on carbon in catalysis were investigated.•Ketone groups (CO) are the oxygen groups for peroxymonosulfate (PMS) activation.•Density functional theory calculations proved the dissociation of PMS by CO.

The active sites for metal-free carbocatalysis in environmental remediation are intricate compared to those for traditional metal-based catalysis. In this study, we report a facile fabrication of amorphous carbon spheres with varying oxygen functional groups by hydrothermal treatment of glucose solutions. With air/N2 annealing and regeneration in the glucose solution of the as-synthesized carbon spheres, the concentrations of oxygen-containing groups were tailored on the amorphous carbon spheres in an Excess-On-Off-On manner. Accordingly, an Off-On-Off-On catalytic behavior in peroxymonosulfate (PMS) activation using these amorphous carbon spheres was observed. To uncover the mechanism of catalytic activity, electron spin resonance (EPR) spectra were recorded to investigate the variation of the generated OH and SO4−radicals. Moreover, density functional theory (DFT) studies were employed to identify the role of oxygen-containing groups on the amorphous carbon spheres in adsorptive OO bond activation of PMS. Results revealed that ketone groups (CO) are the dominant active sites for PMS activation among oxygen-containing functional groups. In order to simulate real wastewater treatment, influences of chloride anions and humic acid on PMS activation for phenol degradation were further evaluated. This study provides an in-depth insight to discovering the role of oxygen-containing functional groups as the active sites in metal-free carbocatalysis.

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Keywords
Active sites; Sulfate radicals; Carbon spheres; DFT; Catalytic oxidation
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Activation of peroxymonosulfate by carbonaceous oxygen groups: experimental and density functional theory calculations
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis B: Environmental - Volume 198, 5 December 2016, Pages 295–302
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
100% Money Back Guarantee
Full-text PDF Download
Online Support
Any Questions? feel free to contact us