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

Abstract

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.

Authors:
 [1];  [1];  [1];  [1];  [2];  [1];  [1]
  1. Tufts Univ., Medford, MA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1223384
Grant/Contract Number:  
AC02-06CH11357; FG02-05ER15730; AC05-00OR22725; SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemical sciences; catalysis; material science; physical chemistry

Citation Formats

Lucci, Felicia R., Liu, Jilei, Marcinkowski, Matthew D., Yang, Ming, Allard, Lawrence F., Flytzani-Stephanopoulos, Maria, and Sykes, E. Charles H. Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit. United States: N. p., 2015. Web. doi:10.1038/ncomms9550.
Lucci, Felicia R., Liu, Jilei, Marcinkowski, Matthew D., Yang, Ming, Allard, Lawrence F., Flytzani-Stephanopoulos, Maria, & Sykes, E. Charles H. Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit. United States. doi:https://doi.org/10.1038/ncomms9550
Lucci, Felicia R., Liu, Jilei, Marcinkowski, Matthew D., Yang, Ming, Allard, Lawrence F., Flytzani-Stephanopoulos, Maria, and Sykes, E. Charles H. Fri . "Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit". United States. doi:https://doi.org/10.1038/ncomms9550. https://www.osti.gov/servlets/purl/1223384.
@article{osti_1223384,
title = {Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit},
author = {Lucci, Felicia R. and Liu, Jilei and Marcinkowski, Matthew D. and Yang, Ming and Allard, Lawrence F. and Flytzani-Stephanopoulos, Maria and Sykes, E. Charles H.},
abstractNote = {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.},
doi = {10.1038/ncomms9550},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {2015},
month = {10}
}

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