Toward rational nanoparticle synthesis: predicting surface intermixing in bimetallic alloy nanocatalysts
Abstract
In this paper, we present a database of first-principles calculated activation energy barriers for two competitive processes involving bimetallic adatom-surface permutations of ten transition metals: (i) adatom “hopping” diffusion and (ii) adatom substitution into the surface. We consider the surface structure sensitivity of these events as well as coverage effects. We find that surface hopping mechanisms are facile and always preferred to substitution events on close-packed fcc(111) and hcp(0001) surfaces. However, surface atom substitution is more facile on the more open fcc(100) surfaces and is competitive with adatom surface hopping, which is more difficult than on the close-packed surfaces. Finally, by comparing the absolute and relative magnitudes of the energetics of hopping and substitution, our calculations can offer qualitative predictions of intermixing and other phenomena relevant to nanocrystal growth, such as the tendency to form intermixed alloys or core–shell structures during layer-by-layer nanoparticle synthesis involving a given bimetallic pair, and thereby inform the rational design and synthesis of novel bimetallic nanomaterials.
- Publication Date:
- Research Org.:
- Univ. of Wisconsin, Madison, WI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Contributing Org.:
- Environmental Molecular Sciences Laboratory (EMSL); the Center for Nanoscale Materials (CNM) at Argonne National Laboratory; and the National Energy Research Scientific Computing Center (NERSC).
- OSTI Identifier:
- 1395996
- Grant/Contract Number:
- FG02-05ER15731
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nanoscale
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 39; Journal ID: ISSN 2040-3364
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY
Citation Formats
Roling, Luke T., and Mavrikakis, Manos. Toward rational nanoparticle synthesis: predicting surface intermixing in bimetallic alloy nanocatalysts. United States: N. p., 2017.
Web. doi:10.1039/C7NR04779G.
Roling, Luke T., & Mavrikakis, Manos. Toward rational nanoparticle synthesis: predicting surface intermixing in bimetallic alloy nanocatalysts. United States. https://doi.org/10.1039/C7NR04779G
Roling, Luke T., and Mavrikakis, Manos. Tue .
"Toward rational nanoparticle synthesis: predicting surface intermixing in bimetallic alloy nanocatalysts". United States. https://doi.org/10.1039/C7NR04779G. https://www.osti.gov/servlets/purl/1395996.
@article{osti_1395996,
title = {Toward rational nanoparticle synthesis: predicting surface intermixing in bimetallic alloy nanocatalysts},
author = {Roling, Luke T. and Mavrikakis, Manos},
abstractNote = {In this paper, we present a database of first-principles calculated activation energy barriers for two competitive processes involving bimetallic adatom-surface permutations of ten transition metals: (i) adatom “hopping” diffusion and (ii) adatom substitution into the surface. We consider the surface structure sensitivity of these events as well as coverage effects. We find that surface hopping mechanisms are facile and always preferred to substitution events on close-packed fcc(111) and hcp(0001) surfaces. However, surface atom substitution is more facile on the more open fcc(100) surfaces and is competitive with adatom surface hopping, which is more difficult than on the close-packed surfaces. Finally, by comparing the absolute and relative magnitudes of the energetics of hopping and substitution, our calculations can offer qualitative predictions of intermixing and other phenomena relevant to nanocrystal growth, such as the tendency to form intermixed alloys or core–shell structures during layer-by-layer nanoparticle synthesis involving a given bimetallic pair, and thereby inform the rational design and synthesis of novel bimetallic nanomaterials.},
doi = {10.1039/C7NR04779G},
journal = {Nanoscale},
number = 39,
volume = 9,
place = {United States},
year = {Tue Sep 19 00:00:00 EDT 2017},
month = {Tue Sep 19 00:00:00 EDT 2017}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 20 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Structurally ordered intermetallic platinum–cobalt core–shell nanoparticles with enhanced activity and stability as oxygen reduction electrocatalysts
journal, October 2012
- Wang, Deli; Xin, Huolin L.; Hovden, Robert
- Nature Materials, Vol. 12, Issue 1, p. 81-87
Collective and single particle diffusion on surfaces
journal, May 2002
- Ala-Nissila, T.; Ferrando, R.; Ying, S. C.
- Advances in Physics, Vol. 51, Issue 3
Shaping binary metal nanocrystals through epitaxial seeded growth
journal, July 2007
- Habas, Susan E.; Lee, Hyunjoo; Radmilovic, Velimir
- Nature Materials, Vol. 6, Issue 9
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Gold Catalysis
journal, December 2006
- Hashmi, A. Stephen K.; Hutchings, Graham J.
- Angewandte Chemie International Edition, Vol. 45, Issue 47
Ru Nanoframes with an fcc Structure and Enhanced Catalytic Properties
journal, March 2016
- Ye, Haihang; Wang, Qingxiao; Catalano, Massimo
- Nano Letters, Vol. 16, Issue 4
Diffusion and Seed Shape: Intertwined Parameters in the Synthesis of Branched Metal Nanostructures
journal, July 2014
- Weiner, Rebecca G.; DeSantis, Christopher J.; Cardoso, Mariana B. T.
- ACS Nano, Vol. 8, Issue 8
Tackling CO Poisoning with Single-Atom Alloy Catalysts
journal, May 2016
- Liu, Jilei; Lucci, Felicia R.; Yang, Ming
- Journal of the American Chemical Society, Vol. 138, Issue 20
Remarkably Selective Iridium Catalysts for the Elaboration of Aromatic C-H Bonds
journal, November 2001
- Cho, J. -Y.
- Science, Vol. 295, Issue 5553
Real-Time Ab Initio KMC Simulation of the Self-Assembly and Sintering of Bimetallic Epitaxial Nanoclusters: Au + Ag on Ag(100)
journal, June 2014
- Han, Yong; Liu, Da-Jiang; Evans, James W.
- Nano Letters, Vol. 14, Issue 8
Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces
journal, February 2014
- Chen, C.; Kang, Y.; Huo, Z.
- Science, Vol. 343, Issue 6177
Atom-Resolved Imaging of Dynamic Shape Changes in Supported Copper Nanocrystals
journal, March 2002
- Hansen, P. L.
- Science, Vol. 295, Issue 5562
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Size and Shape Control of Metal Nanoparticles for Reaction Selectivity in Catalysis
journal, August 2012
- An, Kwangjin; Somorjai, Gabor A.
- ChemCatChem, Vol. 4, Issue 10
Synthesis and Characterization of Ru Cubic Nanocages with a Face-Centered Cubic Structure by Templating with Pd Nanocubes
journal, August 2016
- Zhao, Ming; Figueroa-Cosme, Legna; Elnabawy, Ahmed O.
- Nano Letters, Vol. 16, Issue 8
Atomistic Mechanism of Surfactant-Assisted Epitaxial Growth
journal, July 1998
- Camarero, J.; Ferrón, J.; Cros, V.
- Physical Review Letters, Vol. 81, Issue 4
A Simple Rule of Thumb for Diffusion on Transition-Metal Surfaces
journal, October 2006
- Nilekar, Anand Udaykumar; Greeley, Jeff; Mavrikakis, Manos
- Angewandte Chemie International Edition, Vol. 45, Issue 42
Modeling the Migration of Platinum Nanoparticles on Surfaces Using a Kinetic Monte Carlo Approach
journal, February 2017
- Li, Lin; Plessow, Philipp N.; Rieger, Michael
- The Journal of Physical Chemistry C, Vol. 121, Issue 8
Significant Quantum Effects in Hydrogen Activation
journal, April 2014
- Kyriakou, Georgios; Davidson, Erlend R. M.; Peng, Guowen
- ACS Nano, Vol. 8, Issue 5
Nanoalloys: From Theory to Applications of Alloy Clusters and Nanoparticles
journal, March 2008
- Ferrando, Riccardo; Jellinek, Julius; Johnston, Roy L.
- Chemical Reviews, Vol. 108, Issue 3, p. 845-910
A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000
- Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
A balancing act: manipulating reactivity of shape-controlled metal nanocatalysts through bimetallic architecture
journal, January 2016
- Laskar, M.; Skrabalak, S. E.
- Journal of Materials Chemistry A, Vol. 4, Issue 18
Ab Initio Thermodynamics and Kinetics for Coalescence of Two-Dimensional Nanoislands and Nanopits on Metal (100) Surfaces
journal, September 2016
- Han, Yong; Stoldt, Conrad R.; Thiel, Patricia A.
- The Journal of Physical Chemistry C, Vol. 120, Issue 38
H 2 Activation and Spillover on Catalytically Relevant Pt–Cu Single Atom Alloys
journal, August 2015
- Lucci, Felicia R.; Marcinkowski, Matthew D.; Lawton, Timothy J.
- The Journal of Physical Chemistry C, Vol. 119, Issue 43
Scaling of hopping self-diffusion barriers on fcc(100) surfaces with bulk bond energies
journal, March 1999
- Feibelman, Peter J.
- Surface Science, Vol. 423, Issue 2-3
Direct hydrogenolysis of glycerol into 1,3-propanediol over rhenium-modified iridium catalyst
journal, June 2010
- Nakagawa, Yoshinao; Shinmi, Yasunori; Koso, Shuichi
- Journal of Catalysis, Vol. 272, Issue 2
Trends in the structure and bonding of noble metal clusters
journal, October 2004
- Fernández, Eva M.; Soler, José M.; Garzón, Ignacio L.
- Physical Review B, Vol. 70, Issue 16
Shape-Controlled Synthesis of Metal Nanocrystals: Simple Chemistry Meets Complex Physics?
journal, December 2008
- Xia, Younan; Xiong, Yujie; Lim, Byungkwon
- Angewandte Chemie International Edition, Vol. 48, Issue 1, p. 60-103
Preparation and Optical Aborption Spectra of Au c ore Pt s hell and Pt c ore Au s hell Colloidal Nanoparticles in Aqueous Solution
journal, March 2000
- Henglein, Arnim
- The Journal of Physical Chemistry B, Vol. 104, Issue 10
Surface segregation energies in low-index open surfaces of bimetallic transition metal alloys
journal, January 2009
- Nilekar, Anand Udaykumar; Ruban, Andrei V.; Mavrikakis, Manos
- Surface Science, Vol. 603, Issue 1
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Numerical study of hetero-adsorption and diffusion on (100) and (110) surfaces of Cu, Ag and Au
journal, May 2015
- Elkoraychy, E.; Sbiaai, K.; Mazroui, M.
- Surface Science, Vol. 635
Chemical Routes for the Transformation of Biomass into Chemicals
journal, June 2007
- Corma, Avelino; Iborra, Sara; Velty, Alexandra
- Chemical Reviews, Vol. 107, Issue 6, p. 2411-2502
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Core–Shell Nanostructured Catalysts
journal, December 2012
- Zhang, Qiao; Lee, Ilkeun; Joo, Ji Bong
- Accounts of Chemical Research, Vol. 46, Issue 8
Seed-Mediated Growth of Colloidal Metal Nanocrystals
journal, December 2016
- Xia, Younan; Gilroy, Kyle D.; Peng, Hsin-Chieh
- Angewandte Chemie International Edition, Vol. 56, Issue 1
Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992
- Perdew, John P.; Wang, Yue
- Physical Review B, Vol. 45, Issue 23, p. 13244-13249
Bimetallic Palladium−Gold Nanostructures: Application in Ethanol Oxidation
journal, August 2009
- Ksar, Fayçal; Ramos, Laurence; Keita, Bineta
- Chemistry of Materials, Vol. 21, Issue 15
Synthesis of Bimetallic Au@Pt Nanoparticles with Au Core and Nanostructured Pt Shell toward Highly Active Electrocatalysts
journal, December 2010
- Ataee-Esfahani, Hamed; Wang, Liang; Nemoto, Yoshihiro
- Chemistry of Materials, Vol. 22, Issue 23
Adsorbate-substrate and adsorbate-adsorbate interactions of Na and K adlayers on Al(111)
journal, December 1992
- Neugebauer, Jörg; Scheffler, Matthias
- Physical Review B, Vol. 46, Issue 24
On the role of surface diffusion in determining the shape or morphology of noble-metal nanocrystals
journal, April 2013
- Xia, X.; Xie, S.; Liu, M.
- Proceedings of the National Academy of Sciences, Vol. 110, Issue 17
Platinum-based nanocages with subnanometer-thick walls and well-defined, controllable facets
journal, July 2015
- Zhang, L.; Roling, L. T.; Wang, X.
- Science, Vol. 349, Issue 6246
Molecular Interactions Driving the Layer-by-Layer Assembly of Multilayers
journal, August 2014
- Borges, João; Mano, João F.
- Chemical Reviews, Vol. 114, Issue 18
A Simple Rule of Thumb for Diffusion on Transition-Metal Surfaces
journal, October 2006
- Nilekar, Anand Udaykumar; Greeley, Jeff; Mavrikakis, Manos
- Angewandte Chemie, Vol. 118, Issue 42
Chemical Routes for the Transformation of Biomass into Chemicals
journal, September 2007
- Corma, Avelino; Iborra, Sara; Velty, Alexandra
- ChemInform, Vol. 38, Issue 36
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets
journal, May 2021
- Chen, Ruyi; Cui, Qirui; Liao, Liyang
- Nature Communications, Vol. 12, Issue 1
High-resolution X-ray luminescence extension imaging
journal, February 2021
- Ou, Xiangyu; Qin, Xian; Huang, Bolong
- Nature, Vol. 590, Issue 7846
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020
- Tatemizo, Nobuyuki; Imada, Saki; Okahara, Kizuna
- Scientific Reports, Vol. 10, Issue 1
Gold Catalysis
journal, March 2007
- Hashmi, A. Stephen K.; Hutchings, Graham J.
- ChemInform, Vol. 38, Issue 12
Preparation and Optical Aborption Spectra of Au core Pt shell and Pt core Au shell Colloidal Nanoparticles in Aqueous Solution
journal, February 2000
- Henglein, Arnim
- The Journal of Physical Chemistry B, Vol. 104, Issue 10
Surface Self-Diffusion on Pt(001) by an Atomic Exchange Mechanism
journal, August 1990
- Kellogg, G. L.; Feibelman, Peter J.
- Physical Review Letters, Vol. 65, Issue 7
Works referencing / citing this record:
Shape‐Controlled Synthesis of Colloidal Metal Nanocrystals by Replicating the Surface Atomic Structure on the Seed
journal, April 2018
- Gilroy, Kyle D.; Yang, Xuan; Xie, Shuifen
- Advanced Materials, Vol. 30, Issue 25
Iridium‐Based Cubic Nanocages with 1.1‐nm‐Thick Walls: A Highly Efficient and Durable Electrocatalyst for Water Oxidation in an Acidic Medium
journal, March 2019
- Zhu, Jiawei; Chen, Zitao; Xie, Minghao
- Angewandte Chemie, Vol. 131, Issue 22
Iridium‐Based Cubic Nanocages with 1.1‐nm‐Thick Walls: A Highly Efficient and Durable Electrocatalyst for Water Oxidation in an Acidic Medium
journal, May 2019
- Zhu, Jiawei; Chen, Zitao; Xie, Minghao
- Angewandte Chemie International Edition, Vol. 58, Issue 22
A coordination-based model for transition metal alloy nanoparticles
journal, January 2019
- Roling, Luke T.; Choksi, Tej S.; Abild-Pedersen, Frank
- Nanoscale, Vol. 11, Issue 10