Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit

Lucci, Felicia R.; Liu, Jilei; Marcinkowski, Matthew D.; Yang, Ming; Allard, Lawrence F.; Flytzani-Stephanopoulos, Maria; Sykes, E. Charles H.

doi:10.1038/ncomms9550

Title: Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit

Journal Article · Fri Oct 09 00:00:00 EDT 2015 · Nature Communications

DOI:https://doi.org/10.1038/ncomms9550· OSTI ID:1223384

Lucci, Felicia R. ^[1]; Liu, Jilei ^[1]; Marcinkowski, Matthew D. ^[1]; Yang, Ming ^[1]; Allard, Lawrence F. ^[2]; Flytzani-Stephanopoulos, Maria ^[1]; Sykes, E. Charles H. ^[1]

Tufts Univ., Medford, MA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Platinum is ubiquitous in the production sectors of chemicals and fuels; however, its scarcity in nature and high price will limit future proliferation of platinum-catalysed reactions. One definite approach to conserve platinum involves understanding the smallest number of platinum atoms needed to catalyse a reaction, then designing catalysts with the minimal platinum ensembles. Here we design and test a new generation of platinum–copper nanoparticle catalysts for the selective hydrogenation of 1,3-butadiene,, an industrially important reaction. Isolated platinum atom geometries enable hydrogen activation and spillover but are incapable of C–C bond scission that leads to loss of selectivity and catalyst deactivation. γ-Alumina-supported single-atom alloy nanoparticle catalysts with <1 platinum atom per 100 copper atoms are found to exhibit high activity and selectivity for butadiene hydrogenation to butenes under mild conditions, demonstrating transferability from the model study to the catalytic reaction under practical conditions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: AC02-06CH11357; FG02-05ER15730; AC05-00OR22725; SC00112704

OSTI ID:: 1223384

Journal Information:: Nature Communications, Vol. 6; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 432 works

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Stabilizing a Platinum ₁ Single-Atom Catalyst on Supported Phosphomolybdic Acid without Compromising Hydrogenation Activity Zhang, Bin; Asakura, Hiroyuki; Zhang, Jia Angewandte Chemie, Vol. 128, Issue 29 https://doi.org/10.1002/ange.201602801	journal	May 2016
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Atomically Dispersed Copper-Platinum Dual Sites Alloyed with Palladium Nanorings Catalyze the Hydrogen Evolution Reaction Chao, Tingting; Luo, Xuan; Chen, Wenxing Angewandte Chemie International Edition, Vol. 56, Issue 50 https://doi.org/10.1002/anie.201709803	journal	November 2017
Stabilizing a Platinum ₁ Single-Atom Catalyst on Supported Phosphomolybdic Acid without Compromising Hydrogenation Activity Zhang, Bin; Asakura, Hiroyuki; Zhang, Jia Angewandte Chemie International Edition, Vol. 55, Issue 29 https://doi.org/10.1002/anie.201602801	journal	May 2016
Stabilization of Single Metal Atoms on Graphitic Carbon Nitride Javier, Perez-Ramirez,; Zupeng, Chen,; Sharon, Mitchell, ETH Zurich https://doi.org/10.3929/ethz-b-000128087	text	January 2017
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Title: Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit

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