Tuning the electronic properties of single atom catalysts(SACs)between the central metal and the neighboring surface atoms has emerged as an efficient strategy to boost catalytic efficiency and metal utilization.Here ...Tuning the electronic properties of single atom catalysts(SACs)between the central metal and the neighboring surface atoms has emerged as an efficient strategy to boost catalytic efficiency and metal utilization.Here we describe a simple and efficient approach to create atomically dispersed palladium atoms supported over defect-containing porous ceria nanorod containing palladium up to 0.26 wt.%.The existence of singly dispersed palladium atoms is confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurements.This catalyst shows excellent efficiency in hydrodehalogenation reactions at low H2 pressure under mild conditions,along with satisfactory recyclability and scalability.Density functional theory(DFT)calculations reveal that the high activity stems from the spatial isolation of palladium atoms and the modified electronic structure of palladium confined in defect-containing ceria nanorod.This work may lay the foundation for the facile creation of single atom catalysts within the synthetic community and shed light on the possibility for scale-up production.展开更多
基金the China Postdoctoral Science Foundation(Nos.2019M661247 and 2020T130091)Postdoctoral Science Foundation of Heilongjiang Province(No.LBH-Z19047)+1 种基金Program for Overseas Talents Introduction of Northeast Petroleum University(No.15041260303)Scientific Research Foundation for Returned Scholars of Heilongjiang Province of China(No.719900091).
文摘Tuning the electronic properties of single atom catalysts(SACs)between the central metal and the neighboring surface atoms has emerged as an efficient strategy to boost catalytic efficiency and metal utilization.Here we describe a simple and efficient approach to create atomically dispersed palladium atoms supported over defect-containing porous ceria nanorod containing palladium up to 0.26 wt.%.The existence of singly dispersed palladium atoms is confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurements.This catalyst shows excellent efficiency in hydrodehalogenation reactions at low H2 pressure under mild conditions,along with satisfactory recyclability and scalability.Density functional theory(DFT)calculations reveal that the high activity stems from the spatial isolation of palladium atoms and the modified electronic structure of palladium confined in defect-containing ceria nanorod.This work may lay the foundation for the facile creation of single atom catalysts within the synthetic community and shed light on the possibility for scale-up production.
