Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C-H activation

The recent availability of shale gas has led to a renewed interest in C-H bond activation as the first step towards the synthesis of fuels and fine chemicals. Heterogeneous catalysts based on Ni and Pt can perform this chemistry, but deactivate easily due to coke formation. Cu-based catalysts are no...

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Bibliographic Details
Published in:Nature chemistry 2018-03, Vol.10 (3), p.325-332
Main Authors: Marcinkowski, Matthew D, Darby, Matthew T, Liu, Jilei, Wimble, Joshua M, Lucci, Felicia R, Lee, Sungsik, Michaelides, Angelos, Flytzani-Stephanopoulos, Maria, Stamatakis, Michail, Sykes, E Charles H
Format: Article
Language:English
Subjects:
Activation
Adsorbates
Alloy systems
Alloys
Butane
Catalysis
Catalysts
Chemical bonds
Chemical synthesis
Coke
Coking
Copper
Deactivation
Dilution
Fine chemicals
Hydrogen bonds
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
MATERIALS SCIENCE
Platinum
Shale
Shale gas
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Summary:The recent availability of shale gas has led to a renewed interest in C-H bond activation as the first step towards the synthesis of fuels and fine chemicals. Heterogeneous catalysts based on Ni and Pt can perform this chemistry, but deactivate easily due to coke formation. Cu-based catalysts are not practical due to high C-H activation barriers, but their weaker binding to adsorbates offers resilience to coking. Using Pt/Cu single-atom alloys (SAAs), we examine C-H activation in a number of systems including methyl groups, methane and butane using a combination of simulations, surface science and catalysis studies. We find that Pt/Cu SAAs activate C-H bonds more efficiently than Cu, are stable for days under realistic operating conditions, and avoid the problem of coking typically encountered with Pt. Pt/Cu SAAs therefore offer a new approach to coke-resistant C-H activation chemistry, with the added economic benefit that the precious metal is diluted at the atomic limit.
ISSN:1755-4330
1755-4349
DOI:10.1038/nchem.2915