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Transformation of Bulk Pd to Pd Cations in Small-Pore CHA Zeolites Facilitated by NO.

ABSTRACT: Atomic dispersion of metal species has attracted attention as a unique phenomenon that affects adsorption properties and catalytic activities and that can be used to design so-called single atom materials. In this work, we describe atomic dispersion of bulk Pd into small pores of CHA zeolites. Under 4% NO flow at 600 °C, bulk Pd metal on the outside of CHA zeolites effectively disperses, affording Pd²⁺ cations on Al sites with concomitant formation of N₂O, as revealed by microscopic and spectroscopic characterizations combined with mass spectroscopy. In the present method, even commercially available submicrosized Pd black can be used as a Pd source, and importantly, 4.1 wt % of atomic Pd²⁺ cations, which is the highest loading amount reported so far, can be introduced into CHA zeolites. The structural evolution of bulk Pd metal is also investigated by in situ X-ray absorption spectroscopy (XAS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), as well as ab initio thermodynamic analysis using density functional theory (DFT) calculations.

SUBMITTER: Yasumura S

PROVIDER: S-EPMC8395613 | biostudies-literature |

REPOSITORIES: biostudies-literature

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