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Regulating Crystal Facets of MnO₂ for Enhancing Peroxymonosulfate Activation to Degrade Pollutants: Performance and Mechanism

Fu, J, Gao, P, Wang, L, Zhang, Y, Deng, Y, Huang, R, Zhao, Shuaifei, Yu, Z, Wei, Y, Wang, G and Zhou, S 2022, Regulating Crystal Facets of MnO₂ for Enhancing Peroxymonosulfate Activation to Degrade Pollutants: Performance and Mechanism, Catalysts, vol. 12, no. 3, pp. 1-18, doi: 10.3390/catal12030342.

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Title Regulating Crystal Facets of MnO₂ for Enhancing Peroxymonosulfate Activation to Degrade Pollutants: Performance and Mechanism
Author(s) Fu, J
Gao, P
Wang, L
Zhang, Y
Deng, Y
Huang, R
Zhao, ShuaifeiORCID iD for Zhao, Shuaifei orcid.org/0000-0002-7727-6676
Yu, Z
Wei, Y
Wang, G
Zhou, S
Journal name Catalysts
Volume number 12
Issue number 3
Article ID 342
Start page 1
End page 18
Total pages 18
Publisher MDPI AG
Place of publication Basel, Switzerland
Publication date 2022
ISSN 2073-4344
Keyword(s) Science & Technology
Physical Sciences
Chemistry, Physical
Chemistry
manganese dioxide
surface regulation
peroxymonosulfate activation
nonradical pathway
crystal facet dependence
EFFICIENT PEROXYDISULFATE ACTIVATION
NONRADICAL ACTIVATION
SINGLET OXYGEN
BISPHENOL-A
CATALYTIC-OXIDATION
WASTE-WATER
REMOVAL
PERSULFATE
CARBON
GRAPHENE
Summary On the catalyst surface, crystal facets with different surface atom arrangements and diverse physicochemical properties lead to distinct catalytic activity. Acquiring a highly reactive facet through surface regulation is an efficient strategy to promote the oxidative decomposition of wastewater organic pollutants via peroxymonosulfate (PMS) activation. However, the mechanism through which crystal facets affect PMS activation is still unclear. In this study, three facet-engineered α-MnO2 with different exposed facets were prepared via a facile hydrothermal route. The prepared 310-MnO2 exhibited superior PMS activation performance to 100-MnO2 and 110-MnO2. Moreover, the 310-MnO2/PMS oxidative system was active over a wide pH range and highly resistant to interfering substances from wastewater. These advantages of the 310-MnO2/PMS system make it highly promising for practical wastewater treatment. Based on quenching experiments, electron paramagnetic resonance (EPR) analysis, solvent exchange, and electrochemical measurements, mediated electron transfer was found to be the dominant nonradical pathway for p-chloroaniline (PCA) degradation. A sulfhydryl group (-SH) masking experiment showed that the highly exposed Mn atoms on the 310-MnO2 surface were sites of PMS activation. In addition, density functional theory (DFT) calculations confirmed that the dominant {310} facet promoted adsorption/activation of PMS, which favored the formation of more metastable complexes on the α-MnO2 surface. The reaction mechanism obtained here clarifies the relationship between PMS activation and crystal facets. This study provides significant insights into the rational design of high-performance catalysts for efficient water remediation
Language eng
DOI 10.3390/catal12030342
Field of Research 0306 Physical Chemistry (incl. Structural)
HERDC Research category C1 Refereed article in a scholarly journal
Free to Read? Yes
Persistent URL http://hdl.handle.net/10536/DRO/DU:30165253

Document type: Journal Article
Collections: Institute for Frontier Materials
Open Access Collection
GTP Research
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Created: Thu, 24 Mar 2022, 07:20:28 EST

Every reasonable effort has been made to ensure that permission has been obtained for items included in DRO. If you believe that your rights have been infringed by this repository, please contact drosupport@deakin.edu.au.