Surface-Phosphorylated Ceria for Chlorine-Tolerance Catalysis.
Environ Sci Technol
; 58(2): 1369-1377, 2024 Jan 16.
Article
em En
| MEDLINE
| ID: mdl-38048160
ABSTRACT
An improved fundamental understanding of active site structures can unlock opportunities for catalysis from conceptual design to industrial practice. Herein, we present the computational discovery and experimental demonstration of a highly active surface-phosphorylated ceria catalyst that exhibits robust chlorine tolerance for catalysis. Ab initio molecular dynamics (AIMD) calculations and in situ near-ambient pressure X-ray photoelectron spectroscopy (in situ NAP-XPS) identified a predominantly HPO4 active structure on CeO2(110) and CeO2(111) facets at room temperature. Importantly, further elevating the temperature led to a unique hydrogen (H) atom hopping between coordinatively unsaturated oxygen and the adjacent PâO group of HPO4. Such a mobile H on the catalyst surface can effectively quench the chlorine radicals (Clâ¢) via an orientated reaction analogous to hydrogen atom transfer (HAT), enabling the surface-phosphorylated CeO2-supported monolithic catalyst to exhibit both expected activity and stability for over 68 days during a pilot test, catalyzing the destruction of a complex chlorinated volatile organic compound industrial off-gas.
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1
Coleções:
01-internacional
Base de dados:
MEDLINE
Assunto principal:
Oxigênio
/
Cloro
Idioma:
En
Revista:
Environ Sci Technol
Ano de publicação:
2024
Tipo de documento:
Article