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

Abstract

The recent availability of shale gas has led to a renewed interest in C-H bond activation as the first step towards 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 for this chemistry due to high C-H activation barriers, but their weaker binding to adsorbates offers resilience to coking. Utilizing 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.

Authors:
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Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Engineering and Physical Sciences Research Council (EPSRC); European Commission - Community Research and Development Information Service (CORDIS) - Seventh Framework Programme (FP7)
OSTI Identifier:
1426229
DOE Contract Number:
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nature Chemistry; Journal Volume: 10; Journal Issue: 3
Country of Publication:
United States
Language:
English

Citation Formats

Marcinkowski, Matthew D., Darby, Matthew T., Liu, Jilei, Wimble, Joshua M., Lucci, Felicia R., Lee, Sungsik, Michaelides, Angelos, Flytzani-Stephanopoulos, Maria, Stamatakis, Michail, and Sykes, E. Charles H.. Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C–H activation. United States: N. p., 2018. Web. doi:10.1038/NCHEM.2915.
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.. Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C–H activation. United States. doi:10.1038/NCHEM.2915.
Marcinkowski, Matthew D., Darby, Matthew T., Liu, Jilei, Wimble, Joshua M., Lucci, Felicia R., Lee, Sungsik, Michaelides, Angelos, Flytzani-Stephanopoulos, Maria, Stamatakis, Michail, and Sykes, E. Charles H.. Mon . "Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C–H activation". United States. doi:10.1038/NCHEM.2915.
@article{osti_1426229,
title = {Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C–H activation},
author = {Marcinkowski, Matthew D. and Darby, Matthew T. and Liu, Jilei and Wimble, Joshua M. and Lucci, Felicia R. and Lee, Sungsik and Michaelides, Angelos and Flytzani-Stephanopoulos, Maria and Stamatakis, Michail and Sykes, E. Charles H.},
abstractNote = {The recent availability of shale gas has led to a renewed interest in C-H bond activation as the first step towards 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 for this chemistry due to high C-H activation barriers, but their weaker binding to adsorbates offers resilience to coking. Utilizing 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.},
doi = {10.1038/NCHEM.2915},
journal = {Nature Chemistry},
number = 3,
volume = 10,
place = {United States},
year = {Mon Jan 08 00:00:00 EST 2018},
month = {Mon Jan 08 00:00:00 EST 2018}
}