Citation:
Yaxin Chen, Zhiwei Huang, Xiao Gu, Zhen Ma, Jianmin Chen, Xingfu Tang. Top-down synthesis strategies:Maximum noble-metal atom efficiency in catalytic materials[J]. Chinese Journal of Catalysis,
;2017, 38(9): 1588-1596.
doi:
10.1016/S1872-2067(17)62778-5
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Top-down synthesis has been used to prepare catalytic materials with nanometer sizes, but fabri-cating atomically dispersed metal catalysts remains a challenge because surface single metal atoms are prone to aggregation or coalescence. A top-down strategy is used to synthesize atomically dis-persed metal catalysts, based on supported Ag nanoparticles. The changes of the geometric and electronic structures of the Ag atoms during the top-down process are studied using the in situ syn-chrotron X-ray diffraction technique, ex situ X-ray absorption spectroscopy, and transmission elec-tron microscopy. The experimental results, coupled with the density functional theory calculations, demonstrate that the electronic perturbation of the Ag frontier orbitals, induced by the Ag-O inter-actions at the perimeter of the metal-support interface, is the driving force of the top-down process. The top-down synthesis has two important functions:to increase the number of catalytic active sites and to facilitate the study of complex reaction mechanisms (e.g., formaldehyde oxidation) by developing single-site model catalysts.
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