Subnanometer Substructures in Nanoassemblies Formed from Clusters under a Reactive Atmosphere Revealed Using Machine Learning
Abstract
Size-selected clusters, soft-landed on an oxide substrate, is a promising and highly tunable material for heterogeneous catalysis. Agglomeration of the deposited clusters, however, leads to changes in the particle properties and structure. The latter for such cluster assemblies can also be different from that in self standing nanoparticles of similar sizes. To monitor the formation of such complex materials, in situ studies at different length scales are required. Toward that goal, we combined small-angle X-ray scattering (SAXS), X-ray absorption near-edge structure (XANES) spectroscopy, ab initio simulations, and machine learning (artificial neural network) techniques. We detected significant differences between the sizes of particle agglomerates, as probed by SAXS, and the sizes of locally ordered regions, as seen by XANES. We interpret these differences as an evidence for the fractal, grape-cluster-like structure of the agglomerates; thus, XANES and SAXS provide highly complementary structural information. This finding can have a profound effect on our understanding of particle sintering and assembly processes and of structure properties relationship in ultradispersed metal catalysts in reaction conditions.
- Authors:
-
[4];
[5]
- Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
- Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Univ. of Chicago, IL (United States). Inst. for Molecular Engineering
- Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering, and Dept. of Chemistry
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1480971
- Alternate Identifier(s):
- OSTI ID: 1477464
- Report Number(s):
- BNL-209339-2018-JAAM
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- SC0012704; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 37; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Citation Formats
Timoshenko, Janis, Halder, Avik, Yang, Bing, Seifert, Soenke, Pellin, Michael J., Vajda, Stefan, and Frenkel, Anatoly I. Subnanometer Substructures in Nanoassemblies Formed from Clusters under a Reactive Atmosphere Revealed Using Machine Learning. United States: N. p., 2018.
Web. doi:10.1021/acs.jpcc.8b07952.
Timoshenko, Janis, Halder, Avik, Yang, Bing, Seifert, Soenke, Pellin, Michael J., Vajda, Stefan, & Frenkel, Anatoly I. Subnanometer Substructures in Nanoassemblies Formed from Clusters under a Reactive Atmosphere Revealed Using Machine Learning. United States. https://doi.org/10.1021/acs.jpcc.8b07952
Timoshenko, Janis, Halder, Avik, Yang, Bing, Seifert, Soenke, Pellin, Michael J., Vajda, Stefan, and Frenkel, Anatoly I. Sun .
"Subnanometer Substructures in Nanoassemblies Formed from Clusters under a Reactive Atmosphere Revealed Using Machine Learning". United States. https://doi.org/10.1021/acs.jpcc.8b07952. https://www.osti.gov/servlets/purl/1480971.
@article{osti_1480971,
title = {Subnanometer Substructures in Nanoassemblies Formed from Clusters under a Reactive Atmosphere Revealed Using Machine Learning},
author = {Timoshenko, Janis and Halder, Avik and Yang, Bing and Seifert, Soenke and Pellin, Michael J. and Vajda, Stefan and Frenkel, Anatoly I.},
abstractNote = {Size-selected clusters, soft-landed on an oxide substrate, is a promising and highly tunable material for heterogeneous catalysis. Agglomeration of the deposited clusters, however, leads to changes in the particle properties and structure. The latter for such cluster assemblies can also be different from that in self standing nanoparticles of similar sizes. To monitor the formation of such complex materials, in situ studies at different length scales are required. Toward that goal, we combined small-angle X-ray scattering (SAXS), X-ray absorption near-edge structure (XANES) spectroscopy, ab initio simulations, and machine learning (artificial neural network) techniques. We detected significant differences between the sizes of particle agglomerates, as probed by SAXS, and the sizes of locally ordered regions, as seen by XANES. We interpret these differences as an evidence for the fractal, grape-cluster-like structure of the agglomerates; thus, XANES and SAXS provide highly complementary structural information. This finding can have a profound effect on our understanding of particle sintering and assembly processes and of structure properties relationship in ultradispersed metal catalysts in reaction conditions.},
doi = {10.1021/acs.jpcc.8b07952},
journal = {Journal of Physical Chemistry. C},
number = 37,
volume = 122,
place = {United States},
year = {Sun Aug 26 00:00:00 EDT 2018},
month = {Sun Aug 26 00:00:00 EDT 2018}
}
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Works referenced in this record:
Structural Transition of Gold Nanoclusters: From the Golden Cage to the Golden Pyramid
journal, April 2009
- Huang, Wei; Bulusu, Satya; Pal, Rhitankar
- ACS Nano, Vol. 3, Issue 5
Nanosurface Chemistry on Size-Selected Silicon Clusters
journal, May 1991
- Jarrold, M. F.
- Science, Vol. 252, Issue 5009
Structural Transitions in Size-Selected Germanium Cluster Ions
journal, October 1994
- Hunter, J. M.; Fye, J. L.; Jarrold, M. F.
- Physical Review Letters, Vol. 73, Issue 15
Catalysis by clusters with precise numbers of atoms
journal, July 2015
- Tyo, Eric C.; Vajda, Stefan
- Nature Nanotechnology, Vol. 10, Issue 7
Reversing Size-Dependent Trends in the Oxidation of Copper Clusters through Support Effects: Reversing Size-Dependent Trends in the Oxidation of Copper Clusters through Support Effects
journal, December 2017
- Mammen, Nisha; Spanu, Leonardo; Tyo, Eric C.
- European Journal of Inorganic Chemistry, Vol. 2018, Issue 1
Perspective: Size selected clusters for catalysis and electrochemistry
journal, March 2018
- Halder, Avik; Curtiss, Larry A.; Fortunelli, Alessandro
- The Journal of Chemical Physics, Vol. 148, Issue 11
On the Electronic and Atomic Structures of Small Au N - ( N = 4−14) Clusters: A Photoelectron Spectroscopy and Density-Functional Study
journal, August 2003
- Häkkinen, Hannu; Yoon, Bokwon; Landman, Uzi
- The Journal of Physical Chemistry A, Vol. 107, Issue 32
Computational Design of Clusters for Catalysis
journal, April 2018
- Jimenez-Izal, Elisa; Alexandrova, Anastassia N.
- Annual Review of Physical Chemistry, Vol. 69, Issue 1
Catalysis Applications of Size-Selected Cluster Deposition
journal, November 2015
- Vajda, Stefan; White, Michael G.
- ACS Catalysis, Vol. 5, Issue 12
Investigation of size-dependent properties of sub-nanometer palladium clusters encapsulated within a polyamine dendrimer
journal, January 2013
- Kibata, Takayuki; Mitsudome, Takato; Mizugaki, Tomoo
- Chem. Commun., Vol. 49, Issue 2
Cluster size effects
journal, September 1992
- Jortner, Joshua
- Zeitschrift f�r Physik D Atoms, Molecules and Clusters, Vol. 24, Issue 3
Irregular variations in the melting point of size-selected atomic clusters
journal, May 1998
- Schmidt, Martin; Kusche, Robert; von Issendorff, Bernd
- Nature, Vol. 393, Issue 6682
Oxidative Decomposition of Methanol on Subnanometer Palladium Clusters: The Effect of Catalyst Size and Support Composition
journal, May 2010
- Lee, Sungsik; Lee, Byeongdu; Mehmood, Faisal
- The Journal of Physical Chemistry C, Vol. 114, Issue 23
Carbon Dioxide Conversion to Methanol over Size-Selected Cu 4 Clusters at Low Pressures
journal, July 2015
- Liu, Cong; Yang, Bing; Tyo, Eric
- Journal of the American Chemical Society, Vol. 137, Issue 27
Copper Cluster Size Effect in Methanol Synthesis from CO 2
journal, May 2017
- Yang, Bing; Liu, Cong; Halder, Avik
- The Journal of Physical Chemistry C, Vol. 121, Issue 19
Charging Effects on Bonding and Catalyzed Oxidation of CO on Au8 Clusters on MgO
journal, January 2005
- Yoon, Bokwon; Häkkinen, Hannu; Landman, Uzi
- Science, Vol. 307, Issue 5708, p. 403-407
Electronic Structure Controls Reactivity of Size-Selected Pd Clusters Adsorbed on TiO2 Surfaces
journal, November 2009
- Kaden, W. E.; Wu, T.; Kunkel, W. A.
- Science, Vol. 326, Issue 5954
Bimetallic Ag-Pt Sub-nanometer Supported Clusters as Highly Efficient and Robust Oxidation Catalysts
journal, December 2017
- Negreiros, Fabio R.; Halder, Avik; Yin, Chunrong
- Angewandte Chemie International Edition, Vol. 57, Issue 5
Boron Switch for Selectivity of Catalytic Dehydrogenation on Size-Selected Pt Clusters on Al 2 O 3
journal, August 2017
- Ha, Mai-Anh; Baxter, Eric T.; Cass, Ashley C.
- Journal of the American Chemical Society, Vol. 139, Issue 33
Influence of the substrate oxidation state in the growth of copper clusters on Al2O3(0001) surface: a XANES and EXAFS study
journal, January 1995
- Gota, S.; Gautier, M.; Douillard, L.
- Surface Science, Vol. 323, Issue 1-2
Combined TPRx, in situ GISAXS and GIXAS studies of model semiconductor-supported platinum catalysts in the hydrogenation of ethene
journal, January 2010
- Wyrzgol, Sonja A.; Schäfer, Susanne; Lee, Sungsik
- Physical Chemistry Chemical Physics, Vol. 12, Issue 21
Room-Temperature Dynamics of Vanishing Copper Nanoparticles Supported on Silica
journal, March 2017
- Kim, Dohyung; Becknell, Nigel; Yu, Yi
- Nano Letters, Vol. 17, Issue 4
Stability of Platinum Nanoparticles Supported on SiO 2 /Si(111): A High-Pressure X-ray Photoelectron Spectroscopy Study
journal, November 2012
- Porsgaard, Soeren; Merte, Lindsay R.; Ono, Luis K.
- ACS Nano, Vol. 6, Issue 12
Nanoporous Pt with High Surface Area by Reaction-Limited Aggregation of Nanoparticles
journal, March 2009
- Viswanath, B.; Patra, S.; Munichandraiah, N.
- Langmuir, Vol. 25, Issue 5
Cluster Assemblies Produced by Aggregation of Preformed Ag Clusters in Ionic Liquids
journal, March 2018
- Roese, Stefanie; Kononov, Alexander; Timoshenko, Janis
- Langmuir, Vol. 34, Issue 16
Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects
journal, April 2010
- Lei, Y.; Mehmood, F.; Lee, S.
- Science, Vol. 328, Issue 5975, p. 224-228
Reaction Mechanism for Direct Propylene Epoxidation by Alumina-Supported Silver Aggregates: The Role of the Particle/Support Interface
journal, December 2013
- Cheng, Lei; Yin, Chunrong; Mehmood, Faisal
- ACS Catalysis, Vol. 4, Issue 1
New Technique for Investigating Noncrystalline Structures: Fourier Analysis of the Extended X-Ray—Absorption Fine Structure
journal, November 1971
- Sayers, Dale E.; Stern, Edward A.; Lytle, Farrel W.
- Physical Review Letters, Vol. 27, Issue 18
Solving the structure of nanoparticles by multiple-scattering EXAFS analysis
journal, May 1999
- Frenkel, A. I.
- Journal of Synchrotron Radiation, Vol. 6, Issue 3
Solving the 3D structure of metal nanoparticles
journal, January 2007
- Frenkel, Anatoly
- Zeitschrift für Kristallographie - Crystalline Materials, Vol. 222, Issue 11/2007
Modeling the Structure and Composition of Nanoparticles by Extended X-Ray Absorption Fine-Structure Spectroscopy
journal, July 2011
- Frenkel, Anatoly I.; Yevick, Aaron; Cooper, Chana
- Annual Review of Analytical Chemistry, Vol. 4, Issue 1
Applications of extended X-ray absorption fine-structure spectroscopy to studies of bimetallic nanoparticle catalysts
journal, January 2012
- Frenkel, Anatoly I.
- Chemical Society Reviews, Vol. 41, Issue 24
Real-Time Monitoring of Growing Nanoparticles
journal, May 2003
- Renaud, G.
- Science, Vol. 300, Issue 5624
Simultaneous measurement of X-ray small angle scattering, absorption and reactivity: A continuous flow catalysis reactor
journal, September 2011
- Lee, Sungsik; Lee, Byeongdu; Seifert, Soenke
- Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 649, Issue 1
Reactivity of supported platinum nanoclusters studied by in situ GISAXS: clusters stability under hydrogen
journal, October 2006
- Winans, Randall E.; Vajda, Stefan; Ballentine, Gregory E.
- Topics in Catalysis, Vol. 39, Issue 3-4
Inherent Size Effects on XANES of Nanometer Metal Clusters: Size-Selected Platinum Clusters on Silica
journal, December 2016
- Dai, Yang; Gorey, Timothy J.; Anderson, Scott L.
- The Journal of Physical Chemistry C, Vol. 121, Issue 1
Supervised Machine-Learning-Based Determination of Three-Dimensional Structure of Metallic Nanoparticles
journal, October 2017
- Timoshenko, Janis; Lu, Deyu; Lin, Yuewei
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 20
Electrochemical CO2 Reduction on Metal Electrodes
book, January 2008
- Hori, Y.; Vayenas, Constantinos G.; White, Ralph E.
- Modern Aspects of Electrochemistry, p. 89-189
Nanoporous Copper–Silver Alloys by Additive-Controlled Electrodeposition for the Selective Electroreduction of CO 2 to Ethylene and Ethanol
journal, April 2018
- Hoang, Thao T. H.; Verma, Sumit; Ma, Sichao
- Journal of the American Chemical Society, Vol. 140, Issue 17
Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO 2 Electroreduction: Size and Support Effects
journal, April 2018
- Grosse, Philipp; Gao, Dunfeng; Scholten, Fabian
- Angewandte Chemie, Vol. 130, Issue 21
Dynamic behavior of metal nanoparticles for catalysis
journal, June 2018
- Zhou, Yan; Jin, Chuanchuan; Li, Yong
- Nano Today, Vol. 20
Cu-based nanocatalysts for electrochemical reduction of CO2
journal, August 2018
- Xie, Huan; Wang, Tanyuan; Liang, Jiashun
- Nano Today, Vol. 21
Extended X-Ray—Absorption Fine Structure of Small Cu and Ni Clusters: Binding-Energy and Bond-Length Changes with Cluster Size
journal, July 1979
- Apai, G.; Hamilton, J. F.; Stohr, J.
- Physical Review Letters, Vol. 43, Issue 2
Simple theory for the electronic and atomic structure of small clusters
journal, July 1983
- Tománek, D.; Mukherjee, S.; Bennemann, K. H.
- Physical Review B, Vol. 28, Issue 2
Size-controlled synthesis and characterization of thiol-stabilized gold nanoparticles
journal, November 2005
- Frenkel, A. I.; Nemzer, S.; Pister, I.
- The Journal of Chemical Physics, Vol. 123, Issue 18
On surface stress and surface tension
journal, October 1968
- Mays, C. W.; Vermaak, J. S.; Kuhlmann-Wilsdorf, D.
- Surface Science, Vol. 12, Issue 2
Cluster Core-Level Binding-Energy Shifts: The Role of Lattice Strain
journal, July 2004
- Richter, B.; Kuhlenbeck, H.; Freund, H. -J.
- Physical Review Letters, Vol. 93, Issue 2
Size dependence of core and valence binding energies in Pd nanoparticles: Interplay of quantum confinement and coordination reduction
journal, September 2008
- Aruna, I.; Mehta, B. R.; Malhotra, L. K.
- Journal of Applied Physics, Vol. 104, Issue 6
Lattice-strain control of the activity in dealloyed core–shell fuel cell catalysts
journal, April 2010
- Strasser, Peter; Koh, Shirlaine; Anniyev, Toyli
- Nature Chemistry, Vol. 2, Issue 6
Importance of Interatomic Spacing in Catalytic Reduction of Oxygen in Phosphoric Acid
journal, January 1983
- Jalan, V.
- Journal of The Electrochemical Society, Vol. 130, Issue 11
Is there a contraction of the interatomic distance in small metal particles?
journal, June 1990
- Hansen, L. B.; Stoltze, P.; Nørskov, J. K.
- Physical Review Letters, Vol. 64, Issue 26
A New Procedure for Particle Size Determination by EXAFS Based on Molecular Dynamics Simulations
journal, June 1993
- Clausen, B. S.; Grabaek, L.; Topsoe, H.
- Journal of Catalysis, Vol. 141, Issue 2
Determination of metal particle sizes from EXAFS
journal, August 1994
- Clausena, B. S.; Topsøe, H.; Hansen, L. B.
- Catalysis Today, Vol. 21, Issue 1
Probing structural relaxation in nanosized catalysts by combining EXAFS and reverse Monte Carlo methods
journal, February 2017
- Timoshenko, Janis; Frenkel, Anatoly I.
- Catalysis Today, Vol. 280
Limits and Advantages of X-ray Absorption Near Edge Structure for Nanometer Scale Metallic Clusters
journal, November 2003
- Bazin, D.; Rehr, J. J.
- The Journal of Physical Chemistry B, Vol. 107, Issue 45
Small copper clusters studied by x-ray absorption near-edge structure
journal, April 2012
- Oyanagi, H.; Sun, Z. H.; Jiang, Y.
- Journal of Applied Physics, Vol. 111, Issue 8
Parameter-free calculations of X-ray spectra with FEFF9
journal, January 2010
- Rehr, John J.; Kas, Joshua J.; Vila, Fernando D.
- Physical Chemistry Chemical Physics, Vol. 12, Issue 21
Dendrimer-encapsulated nanoparticles: New synthetic and characterization methods and catalytic applications
journal, January 2011
- Myers, V. Sue; Weir, Michael G.; Carino, Emily V.
- Chemical Science, Vol. 2, Issue 9
Self-consistent aspects of x-ray absorption calculations
journal, August 2009
- Bunău, O.; Joly, Y.
- Journal of Physics: Condensed Matter, Vol. 21, Issue 34
Lattice parameters, densities, expansion coefficients and perfection of structure of Cu and of Cu–In α phase
journal, November 1969
- Straumanis, M. E.; Yu, L. S.
- Acta Crystallographica Section A, Vol. 25, Issue 6
Geometrical Characteristics of Regular Polyhedra: Application to EXAFS Studies of Nanoclusters
conference, January 2007
- Glasner, Dana; Frenkel, Anatoly I.
- X-RAY ABSORPTION FINE STRUCTURE - XAFS13: 13th International Conference, AIP Conference Proceedings
Structure of Copper Microclusters Isolated in Solid Argon
journal, May 1986
- Montano, P. A.; Shenoy, G. K.; Alp, E. E.
- Physical Review Letters, Vol. 56, Issue 19
Catalyst Design with Atomic Layer Deposition
journal, February 2015
- O’Neill, Brandon J.; Jackson, David H. K.; Lee, Jechan
- ACS Catalysis, Vol. 5, Issue 3
Atomic layer deposition of ZnO: a review
journal, February 2014
- Tynell, Tommi; Karppinen, Maarit
- Semiconductor Science and Technology, Vol. 29, Issue 4
Analysis of radiation-induced small Cu particle cluster formation in aqueous CuCl2
journal, July 2001
- Jayanetti, Sumedha; Mayanovic, Robert A.; Anderson, Alan J.
- The Journal of Chemical Physics, Vol. 115, Issue 2
Nanoclusters Synthesized by Synchrotron Radiolysis in Concert with Wet Chemistry
journal, November 2014
- Oyanagi, Hiroyuki; Orimoto, Yuuichi; Hayakawa, Kuniko
- Scientific Reports, Vol. 4, Issue 1
Irena : tool suite for modeling and analysis of small-angle scattering
journal, February 2009
- Ilavsky, Jan; Jemian, Peter R.
- Journal of Applied Crystallography, Vol. 42, Issue 2
Control of island morphology by dynamic coalescence of soft-landed clusters
journal, October 2001
- Bréchignac, C.; Cahuzac, Ph.; Carlier, F.
- The European Physical Journal D, Vol. 16, Issue 1
Thermal and chemical nanofractal relaxation
journal, June 2003
- Br�chignac, C.; Cahuzac, Ph.; Carlier, F.
- The European Physical Journal D - Atomic, Molecular and Optical Physics, Vol. 24, Issue 1-3
Thermally induced morphological transition of silver fractals: Thermally induced morphological transition of silver fractals
journal, October 2013
- Solov'yov, Ilia A.; Solov'yov, Andrey V.; Kébaili, Nouari
- physica status solidi (b), Vol. 251, Issue 3
Photoabsorption of Nanoclusters Formed in Helium Droplets: Transition from Compact to Multicenter Aggregation
journal, June 2011
- Loginov, Evgeny; Gomez, Luis F.; Chiang, Naihao
- Physical Review Letters, Vol. 106, Issue 23
Formation of Unusual Copper Clusters in Helium Nanodroplets
journal, April 2013
- Gomez, Luis F.; Loginov, Evgeny; Halder, Avik
- International Journal of Nanoscience, Vol. 12, Issue 02
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journal, March 2019
- Grammatikopoulos, Panagiotis; Sowwan, Mukhles; Kioseoglou, Joseph
- Advanced Theory and Simulations, Vol. 2, Issue 6
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journal, January 2020
- Olekszyszen, Drielly N.; Albuquerque, Brunno L.; Silva, Dagoberto de O.
- Nanoscale, Vol. 12, Issue 2
Surface‐supported cluster catalysis: Ensembles of metastable states run the show
journal, May 2019
- Zandkarimi, Borna; Alexandrova, Anastassia N.
- Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 9, Issue 6
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journal, October 2019
- Liu, Yang; Marcella, Nicholas; Timoshenko, Janis
- The Journal of Chemical Physics, Vol. 151, Issue 16
Machine learning and big scientific data
journal, January 2020
- Hey, Tony; Butler, Keith; Jackson, Sam
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 378, Issue 2166
Automatic oxidation threshold recognition of XAFS data using supervised machine learning
journal, January 2019
- Miyazato, Itsuki; Takahashi, Lauren; Takahashi, Keisuke
- Molecular Systems Design & Engineering, Vol. 4, Issue 5
Machine learning and big scientific data
journal, January 2020
- Hey, Tony; Butler, Keith; Jackson, Sam
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 378, Issue 2166