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Article: Surface-bound radicals generated from cobalt single-atom catalyst: Mechanism of boosting Fenton-like reactions

TitleSurface-bound radicals generated from cobalt single-atom catalyst: Mechanism of boosting Fenton-like reactions
Authors
KeywordsCV-EQCM
Fenton-like reactions
Peroxymonosulfate
Single-atom catalyst
Surface-bound radicals
Issue Date1-Apr-2023
PublisherElsevier
Citation
Chemical Engineering Journal, 2023, v. 461 How to Cite?
AbstractSurface-bound radicals have been reported to be emerging crucial reactive species in Fenton-like reactions for environmental treatment. However, their identification on catalyst surface and contribution to pollutant degradation have never been well addressed. In this study, single Co atom anchored on Al-doped SiO2 (Co@Al-SiO2) catalyst was well designed for peroxymonosulfate (PMS) activation to produce a high concentration of surface-bound sulfate radicals (SO4[rad]−) and reached 100 % removal percentage of antibiotics, dyes and volatile organic compounds (VOCs) pollutants within several minutes. In-situ cyclic voltammetry-electrochemical quartz crystal microbalance (CV-EQCM) and the derived calculation method were firstly employed to quantitatively identify the surface-bound SO4[rad]−. Results show that abundant surface-bound SO4[rad]− was generated on Co-Si bond and its concentration reached 1.17 × 10−6 mol/m2, which was very close to the theoretical maximum (1.34 × 10−6 mol/m2). Further experiments demonstrated that Co atoms can provide rich binding sites for SO4[rad]−, resulting in the enrichment of surface-bound SO4[rad]− in nanoscale surface. This behavior can remarkably boost the degradation kinetics towards various organic contaminants. Coupled with a membrane in water treatment, this system showed an outstanding performance for degradation of pollutants such as dyes (>99 %) with the flow rate of 20 ml/min after 0.5 s, which was considerably faster than traditional treatments. This study provides a fundamental insight into surface-bound radical, guiding the rational design of catalyst for Fenton-like reactions in environmental application.
Persistent Identifierhttp://hdl.handle.net/10722/328512
ISSN
2023 Impact Factor: 13.3
2023 SCImago Journal Rankings: 2.852
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorXie, R-
dc.contributor.authorGuo, K-
dc.contributor.authorAo, Z-
dc.contributor.authorSuo, Z-
dc.contributor.authorHuang, H-
dc.contributor.authorLeung, DYC-
dc.date.accessioned2023-06-28T04:45:37Z-
dc.date.available2023-06-28T04:45:37Z-
dc.date.issued2023-04-01-
dc.identifier.citationChemical Engineering Journal, 2023, v. 461-
dc.identifier.issn1385-8947-
dc.identifier.urihttp://hdl.handle.net/10722/328512-
dc.description.abstractSurface-bound radicals have been reported to be emerging crucial reactive species in Fenton-like reactions for environmental treatment. However, their identification on catalyst surface and contribution to pollutant degradation have never been well addressed. In this study, single Co atom anchored on Al-doped SiO2 (Co@Al-SiO2) catalyst was well designed for peroxymonosulfate (PMS) activation to produce a high concentration of surface-bound sulfate radicals (SO4[rad]−) and reached 100 % removal percentage of antibiotics, dyes and volatile organic compounds (VOCs) pollutants within several minutes. In-situ cyclic voltammetry-electrochemical quartz crystal microbalance (CV-EQCM) and the derived calculation method were firstly employed to quantitatively identify the surface-bound SO4[rad]−. Results show that abundant surface-bound SO4[rad]− was generated on Co-Si bond and its concentration reached 1.17 × 10−6 mol/m2, which was very close to the theoretical maximum (1.34 × 10−6 mol/m2). Further experiments demonstrated that Co atoms can provide rich binding sites for SO4[rad]−, resulting in the enrichment of surface-bound SO4[rad]− in nanoscale surface. This behavior can remarkably boost the degradation kinetics towards various organic contaminants. Coupled with a membrane in water treatment, this system showed an outstanding performance for degradation of pollutants such as dyes (>99 %) with the flow rate of 20 ml/min after 0.5 s, which was considerably faster than traditional treatments. This study provides a fundamental insight into surface-bound radical, guiding the rational design of catalyst for Fenton-like reactions in environmental application.-
dc.languageeng-
dc.publisherElsevier-
dc.relation.ispartofChemical Engineering Journal-
dc.subjectCV-EQCM-
dc.subjectFenton-like reactions-
dc.subjectPeroxymonosulfate-
dc.subjectSingle-atom catalyst-
dc.subjectSurface-bound radicals-
dc.titleSurface-bound radicals generated from cobalt single-atom catalyst: Mechanism of boosting Fenton-like reactions-
dc.typeArticle-
dc.identifier.doi10.1016/j.cej.2023.141920-
dc.identifier.scopuseid_2-s2.0-85148381500-
dc.identifier.volume461-
dc.identifier.isiWOS:000944569100001-
dc.identifier.issnl1385-8947-

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