Surface-Phosphorylated Ceria for Chlorine-Tolerance Catalysis.
Yuetan SuKexin CaoYunhao LuQingjie MengQiguang DaiXueqing LuoHanfeng LuZhongbiao WuXiaole WengPublished in: Environmental science & technology (2023)
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 HPO 4 active structure on CeO 2 (110) and CeO 2 (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 P═O group of HPO 4 . Such a mobile H on the catalyst surface can effectively quench the chlorine radicals (Cl • ) via an orientated reaction analogous to hydrogen atom transfer (HAT), enabling the surface-phosphorylated CeO 2 -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.
Keyphrases
- room temperature
- molecular dynamics
- visible light
- ionic liquid
- density functional theory
- drinking water
- high resolution
- wastewater treatment
- primary care
- small molecule
- heavy metals
- healthcare
- highly efficient
- carbon dioxide
- randomized controlled trial
- magnetic resonance imaging
- computed tomography
- particulate matter
- metal organic framework
- study protocol
- water soluble
- molecularly imprinted