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Catalytic ozonation not relying on hydroxyl radical oxidation: A selective and competitive reaction process related to metal–carboxylate complexes

Paper ID Volume ID Publish Year Pages File Format Full-Text
45423 46410 2014 9 PDF Available
Title
Catalytic ozonation not relying on hydroxyl radical oxidation: A selective and competitive reaction process related to metal–carboxylate complexes
Abstract

•Non-hydroxyl radical related catalytic ozonation.•High activity of the catalyst at neutral pH.•Activity related to surface metal–carboxylate complex structures.•Selective and competitive degradation of carboxylates.•Competitive adsorption of carboxylates.

Catalytic ozonation following non-hydroxyl radical pathway is an important technique not only to degrade refractory carboxylic-containing organic compounds/matter but also to avoid catalyst deactivation caused by metal–carboxylate complexation. It is unknown whether this process is effective for all carboxylates or selective to special molecule structures. In this work, the selectivity was confirmed using O3/(CuO/CeO2) and six distinct ozone-resistant probe carboxylates (i.e., acetate, citrate, malonate, oxalate, pyruvate and succinate). Among these probe compounds, pyruvate, oxalate, and citrate were readily degraded following the rate order of oxalate > citrate > pyruvate, while the degradation of acetate, malonate, and succinate was not promoted. The selectivity was independent on carboxylate group number of the probe compounds and solution pH. Competitive degradation was observed for carboxylate mixtures following the preference order of citrate, oxalate, and finally pyruvate. The competitive degradation was ascribed to competitive adsorption on the catalyst surface. It was revealed that the catalytically degradable compounds formed bidentate chelating or bridging complexes with surface copper sites of the catalyst, i.e., the active sites. The catalytically undegradable carboxylates formed monodentate complexes with surface copper sites or just electrostatically adsorbed on the catalyst surface. The selectivity, relying on the structure of surface metal–carboxylate complex, should be considered in the design of catalytic ozonation process.

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Keywords
Catalytic ozonation; Selectivity; Competitive degradation; Competitive adsorption; Metal–carboxylate complex structure
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis B: Environmental - Volume 144, January 2014, Pages 831–839
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