Deep Oxidation of Chlorinated VOCs by Efficient Catalytic Peroxide Activation over Nanoconfined Co@NCNT Catalysts

The catalytic removal of chlorinated VOCs (CVOCs) in gas–solid reactions usually suffers from chlorine-containing byproduct formation and catalyst deactivation. AOP wet scrubber has recently attracted ever-increasing interest in VOC treatment due to its advantages of high efficiency and no gaseous b...

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Bibliographic Details
Published in:Environmental science & technology 2024-01, Vol.58 (3), p.1625-1635
Main Authors: Xie, Xiaowen, Xiao, Fei, Zhan, Sihui, Zhu, Mingshan, Xiang, Yongjie, Zhong, Huanran, Huang, Haibao
Format: Article
Language:English
Subjects:
Byproducts
Carbon dioxide
Carbon nanotubes
Catalysts
Catalytic activity
Chemical reactions
Chlorine
Chlorobenzene
Cobalt
Exhaust gases
Gas-solid reactions
Nanoparticles
Occurrence, Fate, and Transport of Contaminants in Indoor Air and Atmosphere
Oxidation
Recyclability
Redox properties
Scrubbers
VOCs
Volatile organic compounds
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Summary:The catalytic removal of chlorinated VOCs (CVOCs) in gas–solid reactions usually suffers from chlorine-containing byproduct formation and catalyst deactivation. AOP wet scrubber has recently attracted ever-increasing interest in VOC treatment due to its advantages of high efficiency and no gaseous byproduct emission. Herein, the low-valence Co nanoparticles (NPs) confined in a N-doped carbon nanotube (Co@NCNT) were studied to activate peroxymonosulfate (PMS) for efficient CVOC removal in a wet scrubber. Co@NCNT exhibited unprecedented catalytic activity, recyclability, and low Co ion leakage (0.19 mg L–1) for chlorobenzene degradation in a very wide pH range (3–11). The chlorobenzene removal efficiency was kept stable above 90% over Co@NCNT, much higher than that of nonconfined Co@NCNS (45%). The low-valence Co NPs achieved a continuous electron redox cycling (Co0/Co2+ → Co3+ → Co0/Co2+) and greatly promoted the O–O bond dissociation of PMS with the least energy (0.83 eV) inside the channel of Co@NCNT to form abundant HO• and SO4 •–. Thus, the deep oxidation of chlorobenzene was achieved without any biphenyl byproducts from the coupling reaction. This study provided a new avenue for designing novel nanoconfined catalysts with outstanding activity, paving the way for the deep oxidation of CVOC waste gas via AOP wet scrubber.
ISSN:0013-936X
1520-5851
DOI:10.1021/acs.est.3c08329