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

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.

doi:10.1038/NCHEM.2915

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

Journal Article · Mon Jan 08 00:00:00 EST 2018 · Nature Chemistry

DOI:https://doi.org/10.1038/NCHEM.2915· OSTI ID:1426229

Marcinkowski, Matthew D. ^[1]; Darby, Matthew T. ^[2]; Liu, Jilei ^[3]; Wimble, Joshua M. ^[3]; Lucci, Felicia R. ^[1]; Lee, Sungsik ^[4]; Michaelides, Angelos ^[5]; Flytzani-Stephanopoulos, Maria ^[3]; Stamatakis, Michail ^[6]; ^[1]

Tufts Univ., Medford, MA (United States). Dept. of Chemistry
Univ. College London, London (United Kingdom). Thomas Young Centre and Dept. of Chemical Engineering
Tufts Univ., Medford, MA (United States). Dept. of Chemical and Biological Engineering
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
Univ. College London, London (United Kingdom). Thomas Young Centre, London Centre for Nanotechnology and Dept. of Physics and Astronomy
Univ. College London, London (United Kingdom). Thomas Young Centre and Dept. of Chemical Engineering

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)

Sponsoring Organization:: Engineering and Physical Sciences Research Council (EPSRC); European Union (EU); Royal Society; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725; FG02-05ER15730; SC0004738; SC0012573

OSTI ID:: 1426229

Journal Information:: Nature Chemistry, Journal Name: Nature Chemistry Journal Issue: 3 Vol. 10; ISSN 1755-4330

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Dehydrogenation of Propane to Propylene Using Promoter-Free Hierarchical Pt/Silicalite-1 Nanosheets Wannapakdee, Wannaruedee; Yutthalekha, Thittaya; Dugkhuntod, Pannida Catalysts, Vol. 9, Issue 2 https://doi.org/10.3390/catal9020174	journal	February 2019
The Multifaceted Reactivity of Single-Atom Heterogeneous Catalysts Mitchell, Sharon; Vorobyeva, Evgeniya; Pérez-Ramírez, Javier ETH Zurich https://doi.org/10.3929/ethz-b-000304150	text	January 2018
The quantum nature of hydrogen Fang, Wei; Chen, Ji; Feng, Yexin arXiv https://doi.org/10.48550/arxiv.1812.07848	preprint	January 2018

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