Journal
NANOSCALE
Volume 13, Issue 30, Pages 12874-12884Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1nr03055h
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Funding
- National Key Research and Development Program of China [2019YFA0705803]
- National Natural Science Foundation of China [51878643]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21021101]
- Youth Innovation Promotion Association CAS [2020190]
- DICPQIBEBT [DICPQIBEBT UN201809]
- Dalian supports high-level talent innovation and entrepreneurship projects [2018RQ04]
- Dalian Science and Technology Innovation Fund Project [2019J12SN69]
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A series of LaFe1-xMnxO3-delta perovskite nanocatalysts were synthesized and tested for catalytic ozonation of m-cresol for the first time. LaFe0.26Mn0.74O3-delta with a rhombohedral structure showed excellent catalytic performance and structural stability due to abundant oxygen vacancies and higher Fe2+/Fe3+ and Mn3+/Mn4+ ratios, enhancing electron transfer and promoting ROS production. The research not only revealed the adsorption/decomposition pathways of ozone but also provided insight into the electron transfer pathway during the catalytic ozonation process on nanocatalysts.
Here, a series of LaFe1-xMnxO3-delta perovskite nanocatalysts were synthesized and tested for the catalytic ozonation of m-cresol for the first time. The B-site cation is regulated by metal doping, and the resulting LaFe0.26Mn0.74O3-delta with a rhombohedral structure showed excellent catalytic performance and structural stability owing to the abundant oxygen vacancies and the higher Fe2+/Fe3+ and Mn3+/Mn4+ ratios. Theoretical calculations have revealed that the oxygen vacancy has a strong affinity for ozone adsorption, and thus facilitated ozone decomposition by extending the O-O bond. Combined with low-valence Fe2+ and Mn3+ cations, the electron transfer in the catalytic ozonation reaction has been enhanced, which has promoted the production of reactive oxygen species (ROS). Taken together, the degradation pathway of m-cresol was proposed. Additionally, the LaFe0.26Mn0.74O3-delta catalyst remained stable during a 60 h reaction. This study has not only revealed the adsorption/decomposition pathways of ozone using LaFe0.26Mn0.74O3-delta perovskite nanocatalysts but also provided indepth insight into the electron transfer pathway on the surface of nanocatalysts during the process of catalytic ozonation.
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