Publication Date

10-15-2018

Department

Ames Laboratory; Chemical and Biological Engineering

Campus Units

Ames Laboratory, Chemical and Biological Engineering

OSTI ID+

1505166

Report Number

IS-J 9844

DOI

10.1021/jacs.8b08162

Journal Title

Journal of the American Chemical Society

Volume Number

140

Issue Number

44

First Page

14870

Last Page

14877

Abstract

Supported multimetallic nanoparticles (NPs) are widely used in industrial catalytic processes, where the relation between surface structure and function is well-known. However, the effect of subsurface layers on such catalysts remains mostly unstudied. Here, we demonstrate a clear subsurface effect on supported 2 nm core–shell NPs with atomically precise and high temperature stable Pt3Mn intermetallic surface measured by in situ synchrotron X-ray Diffraction, difference X-ray Absorption Spectroscopy, and Energy Dispersive X-ray Spectroscopy. The NPs with a Pt3Mn subsurface have 98% selectivity to C–H over C–C bond activation during propane dehydrogenation at 550 °C compared with 82% for core–shell NPs with a Pt subsurface. The difference is correlated with significant reduction in the heats of reactant adsorption due to the Pt3Mn intermetallic subsurface as discerned by theory as well as experiment. The findings of this work highlight the importance of subsurface for supported NP catalysts, which can be tuned via controlled intermetallic formation. Such approach is generally applicable to modifying multimetallic NPs, adding another dimension to the tunability of their catalytic performance.

DOE Contract Number(s)

AC02-06CH11357

Language

en

Department of Energy Subject Categories

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Publisher

Iowa State University Digital Repository, Ames IA (United States)

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