• Gallington, Leighanne C.
• Farha, Omar K.
• Lercher, Johannes A.
• Ferrandon, Magali
• Chapman, Karena W.
• Zheng, Jian
• Camaioni, Donald M.
• Vjunov, Aleksei
• Fulton, John L.
• Webber, Thomas E.
• Penn, R. Lee
• Platero-Prats, Ana E.
• Getman, Rachel B.
• Pellizzeri, Steven
• Vermeulen, Nicolaas A.
• Martinson, Alex B. F.
• Mavrantonakis, Andreas
• Kim, In Soo
• Li, Zhanyong
• Hupp, Joseph T.

Abstract

<p>Single atoms and few-atom clusters of platinum are uniformly installed on the zirconia nodes of a metal-organic framework (MOF) NU-1000 via targeted vapor-phase synthesis. The catalytic Pt clusters, site-isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 °C. In situ IR spectroscopy reveals the presence of both single atoms and few-atom clusters that depend upon synthesis conditions. Operando X-ray absorption spectroscopy and X-ray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novel catalyst. These results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size-selected clusters, including noble metals, on a high surface area support.</p>

Topics

• density
• impedance spectroscopy
• surface
• cluster
• phase
• theory
• Platinum
• density functional theory
• x-ray absorption spectroscopy
• sintering
• infrared spectroscopy
• atomic layer deposition