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:
-
- Tufts Univ., Medford, MA (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- 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 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. 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. 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 = {Fri Oct 09 00:00:00 EDT 2015},
month = {Fri Oct 09 00:00:00 EDT 2015}
}
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Single-atom catalyst: a rising star for green synthesis of fine chemicals
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Dynamic traction of lattice-confined platinum atoms into mesoporous carbon matrix for hydrogen evolution reaction
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A sulfur-tethering synthesis strategy toward high-loading atomically dispersed noble metal catalysts
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Tuning the Selectivity of Catalytic Carbon Dioxide Hydrogenation over Iridium/Cerium Oxide Catalysts with a Strong Metal-Support Interaction
journal, August 2017
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Atomically Dispersed Copper-Platinum Dual Sites Alloyed with Palladium Nanorings Catalyze the Hydrogen Evolution Reaction
journal, November 2017
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Intermetallic Compounds as an Alternative to Single‐atom Alloy Catalysts: Geometric and Electronic Structures from Advanced X‐ray Spectroscopies and Computational Studies
journal, January 2020
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Insight of the stability and activity of platinum single atoms on ceria
journal, May 2019
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In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation
journal, March 2019
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Platinum–copper single atom alloy catalysts with high performance towards glycerol hydrogenolysis
journal, December 2019
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Heterogeneous single-atom catalysis
journal, May 2018
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Palladium–gold single atom alloy catalysts for liquid phase selective hydrogenation of 1-hexyne
journal, January 2017
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A nickel–iridium alloy as an efficient heterogeneous catalyst for hydrogenation of olefins
journal, January 2019
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Elucidating the composition of PtAg surface alloys with atomic-scale imaging and spectroscopy
journal, October 2019
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Probing structural changes upon carbon monoxide coordination to single metal adatoms
journal, February 2020
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Recent advances in the precise control of isolated single-site catalysts by chemical methods
journal, June 2018
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Stabilization of Single Metal Atoms on Graphitic Carbon Nitride
text, January 2017
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Stabilizing a Platinum 1 Single-Atom Catalyst on Supported Phosphomolybdic Acid without Compromising Hydrogenation Activity
journal, May 2016
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Hydrogen Diffusion Guided Design of Pt‐Based Alloys for Inhibition of Butadiene Over‐Hydrogenation
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Single-atom heterogeneous catalysts based on distinct carbon nitride scaffolds
text, January 2018
- Chen, Z.; Vorobyeva, E.; Mitchell, S.
- Apollo - University of Cambridge Repository
The Multifaceted Reactivity of Single-Atom Heterogeneous Catalysts
text, January 2018
- Mitchell, Sharon; Vorobyeva, Evgeniya; Pérez-Ramírez, Javier
- ETH Zurich
Atomically Dispersed Copper-Platinum Dual Sites Alloyed with Palladium Nanorings Catalyze the Hydrogen Evolution Reaction
journal, November 2017
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Stabilizing a Platinum 1 Single-Atom Catalyst on Supported Phosphomolybdic Acid without Compromising Hydrogenation Activity
journal, May 2016
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Stabilization of Single Metal Atoms on Graphitic Carbon Nitride
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Alloy, Janus and core-shell nanoparticles: Numerical modeling of their nucleation and growth in physical synthesis
text, January 2019
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Silica-Supported Au-Ag Catalysts for the Selective Hydrogenation of Butadiene
journal, June 2017
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Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction
journal, March 2019
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Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst
journal, March 2016
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Thermally stable single atom Pt/m-Al2O3 for selective hydrogenation and CO oxidation
journal, July 2017
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In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation
journal, March 2019
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Isolating contiguous Pt atoms and forming Pt-Zn intermetallic nanoparticles to regulate selectivity in 4-nitrophenylacetylene hydrogenation
journal, August 2019
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Quasi Pd1Ni single-atom surface alloy catalyst enables hydrogenation of nitriles to secondary amines
journal, November 2019
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Platinum–copper single atom alloy catalysts with high performance towards glycerol hydrogenolysis
journal, December 2019
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High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
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Selective hydrogenation of 1,3-butadiene catalyzed by a single Pd atom anchored on graphene: the importance of dynamics
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Dynamic traction of lattice-confined platinum atoms into mesoporous carbon matrix for hydrogen evolution reaction
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A sulfur-tethering synthesis strategy toward high-loading atomically dispersed noble metal catalysts
journal, October 2019
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