Interaction between Single Metal Atoms and UiO-66 Framework Revealed by Low-Dose Imaging.

Nano Lett

Beijing Key Laboratory of Green Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.

Published: March 2023

Atomically dispersed metals encapsulated in metal-organic frameworks (MOFs) have attracted extensive attention in catalysis and energy fields. Amino groups were considered conducive to the formation of single atom catalysts (SACs) due to the strong metal-linker interactions. Here, atomic details of Pt@UiO-66 and Pd@UiO-66-NH are revealed using low-dose integrated differential phase contrast scanning transmission electron microscopy (iDPC-STEM). Single Pt atoms locate on the benzene ring of -benzenedicarboxylic acid (BDC) linkers in Pt@UiO-66, while single Pd atoms are adsorbed by the amino groups in Pd@UiO-66-NH. However, Pt@UiO-66-NH and Pd@UiO-66 show obvious clusters. Therefore, amino groups do not always favor the formation of SACs, and density functional theory (DFT) calculations indicate that a moderate binding strength between metals and MOFs is preferred. These results directly reveal the adsorption sites of single metal atoms in UiO-66 family, paving the way for understanding the interaction between single metal atoms and the MOFs.

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http://dx.doi.org/10.1021/acs.nanolett.2c04569DOI Listing

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