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Title: Evolution of atomic structure during nanoparticle formation

Abstract

Understanding the mechanism of nanoparticle formation during synthesis is a key prerequisite for the rational design and engineering of desirable materials properties, yet remains elusive due to the difficulty of studying structures at the nanoscale under real conditions. Here, the first comprehensive structural description of the formation of a nanoparticle, yttria-stabilized zirconia (YSZ), all the way from its ionic constituents in solution to the final crystal, is presented. The transformation is a complicated multi-step sequence of atomic reorganizations as the material follows the reaction pathway towards the equilibrium product. Prior to nanoparticle nucleation, reagents reorganize into polymeric species whose structure is incompatible with the final product. Instead of direct nucleation of clusters into the final product lattice, a highly disordered intermediate precipitate forms with a local bonding environment similar to the product yet lacking the correct topology. During maturation, bond reforming occurs by nucleation and growth of distinct domains within the amorphous intermediary. The present study moves beyond kinetic modeling by providing detailed real-time structural insight, and it is demonstrated that YSZ nanoparticle formation and growth is a more complex chemical process than accounted for in conventional models. This level of mechanistic understanding of the nanoparticle formation is the firstmore » step towards more rational control over nanoparticle synthesis through control of both solution precursors and reaction intermediaries.« less

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1335051
Grant/Contract Number:  
SC0001085
Resource Type:
Published Article
Journal Name:
IUCrJ
Additional Journal Information:
Journal Name: IUCrJ Journal Volume: 1 Journal Issue: 3; Journal ID: ISSN 2052-2525
Publisher:
International Union of Crystallography (IUCr)
Country of Publication:
United Kingdom
Language:
English

Citation Formats

Tyrsted, Christoffer, Lock, Nina, Jensen, Kirsten M. Ø., Christensen, Mogens, Bøjesen, Espen D., Emerich, Hermann, Vaughan, Gavin, Billinge, Simon J. L., and Iversen, Bo B. Evolution of atomic structure during nanoparticle formation. United Kingdom: N. p., 2014. Web. doi:10.1107/S2052252514006538.
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Tyrsted, Christoffer, Lock, Nina, Jensen, Kirsten M. Ø., Christensen, Mogens, Bøjesen, Espen D., Emerich, Hermann, Vaughan, Gavin, Billinge, Simon J. L., & Iversen, Bo B. Evolution of atomic structure during nanoparticle formation. United Kingdom. https://doi.org/10.1107/S2052252514006538
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Tyrsted, Christoffer, Lock, Nina, Jensen, Kirsten M. Ø., Christensen, Mogens, Bøjesen, Espen D., Emerich, Hermann, Vaughan, Gavin, Billinge, Simon J. L., and Iversen, Bo B. Mon . "Evolution of atomic structure during nanoparticle formation". United Kingdom. https://doi.org/10.1107/S2052252514006538.
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@article{osti_1335051,
title = {Evolution of atomic structure during nanoparticle formation},
author = {Tyrsted, Christoffer and Lock, Nina and Jensen, Kirsten M. Ø. and Christensen, Mogens and Bøjesen, Espen D. and Emerich, Hermann and Vaughan, Gavin and Billinge, Simon J. L. and Iversen, Bo B.},
abstractNote = {Understanding the mechanism of nanoparticle formation during synthesis is a key prerequisite for the rational design and engineering of desirable materials properties, yet remains elusive due to the difficulty of studying structures at the nanoscale under real conditions. Here, the first comprehensive structural description of the formation of a nanoparticle, yttria-stabilized zirconia (YSZ), all the way from its ionic constituents in solution to the final crystal, is presented. The transformation is a complicated multi-step sequence of atomic reorganizations as the material follows the reaction pathway towards the equilibrium product. Prior to nanoparticle nucleation, reagents reorganize into polymeric species whose structure is incompatible with the final product. Instead of direct nucleation of clusters into the final product lattice, a highly disordered intermediate precipitate forms with a local bonding environment similar to the product yet lacking the correct topology. During maturation, bond reforming occurs by nucleation and growth of distinct domains within the amorphous intermediary. The present study moves beyond kinetic modeling by providing detailed real-time structural insight, and it is demonstrated that YSZ nanoparticle formation and growth is a more complex chemical process than accounted for in conventional models. This level of mechanistic understanding of the nanoparticle formation is the first step towards more rational control over nanoparticle synthesis through control of both solution precursors and reaction intermediaries.},
doi = {10.1107/S2052252514006538},
journal = {IUCrJ},
number = 3,
volume = 1,
place = {United Kingdom},
year = {Mon Apr 14 00:00:00 EDT 2014},
month = {Mon Apr 14 00:00:00 EDT 2014}
}
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https://doi.org/10.1107/S2052252514006538
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Works referenced in this record:

Rapid and Continuous Hydrothermal Crystallization of Metal Oxide Particles in Supercritical Water
journal, April 1992

Pulsed supercritical synthesis of anatase TiO2 nanoparticles in a water–isopropanol mixture studied by in situ powder X-ray diffraction
journal, January 2013

  • Eltzholtz, Jakob Rostgaard; Tyrsted, Christoffer; Jensen, Kirsten Marie Ørnsbjerg
  • Nanoscale, Vol. 5, Issue 6
  • DOI: 10.1039/c3nr33127j

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

Time-Resolved In Situ Diffraction Study of the Solvothermal Crystallization of Some Prototypical Metal-Organic Frameworks
journal, December 2009

  • Millange, Franck; Medina, Manuela I.; Guillou, Nathalie
  • Angewandte Chemie International Edition, Vol. 49, Issue 4
  • DOI: 10.1002/anie.200905627

Watching solids crystallise using in situ powder diffraction
journal, January 2000

  • Walton, Richard I.; O’Hare, Dermot
  • Chemical Communications, Issue 23
  • DOI: 10.1039/b007795j

In Situ and Ex Situ Studies of Platinum Nanocrystals: Growth and Evolution in Solution
journal, October 2009

  • Cheong, Soshan; Watt, John; Ingham, Bridget
  • Journal of the American Chemical Society, Vol. 131, Issue 40
  • DOI: 10.1021/ja9065688

The crystal structure of baddeleyite (monoclinic ZrO 2 ) and its relation to the polymorphism of ZrO 2
journal, June 1965

Kinetics and Mechanisms of Aggregative Nanocrystal Growth
journal, September 2013

  • Wang, Fudong; Richards, Vernal N.; Shields, Shawn P.
  • Chemistry of Materials, Vol. 26, Issue 1
  • DOI: 10.1021/cm402139r

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
  • DOI: 10.1039/b926434e

A time-resolved diffraction study of a window of stability in the synthesis of a copper carboxylate metal–organic framework
journal, January 2011

  • Millange, Franck; El Osta, Racha; Medina, Manuela E.
  • CrystEngComm, Vol. 13, Issue 1
  • DOI: 10.1039/C0CE00530D

Nucleation Control of Size and Dispersity in Aggregative Nanoparticle Growth. A Study of the Coarsening Kinetics of Thiolate-Capped Gold Nanocrystals
journal, May 2010

  • Shields, Shawn P.; Richards, Vernal N.; Buhro, William E.
  • Chemistry of Materials, Vol. 22, Issue 10
  • DOI: 10.1021/cm100458b

Kinetics of Phase Change. I General Theory
journal, December 1939

  • Avrami, Melvin
  • The Journal of Chemical Physics, Vol. 7, Issue 12, p. 1103-1112
  • DOI: 10.1063/1.1750380

Oxide-Ion Electrolytes
journal, August 2003

Oxygen-induced structural change of the tetragonal phase around the tetragonal–cubic phase boundary in ZrO 2 –YO 1.5 solid solutions
journal, December 1994

  • Yashima, M.; Sasaki, S.; Kakihana, M.
  • Acta Crystallographica Section B Structural Science, Vol. 50, Issue 6
  • DOI: 10.1107/S0108768194006257

Synthesis of sodium zeolites from a natural halloysite
journal, November 2001

Solvent effect on microstructure of yttria-stabilized zirconia (YSZ) particles in solvothermal synthesis
journal, January 2006

Revealing the Mechanisms behind SnO 2 Nanoparticle Formation and Growth during Hydrothermal Synthesis: An In Situ Total Scattering Study
journal, April 2012

  • Jensen, Kirsten M. Ø.; Christensen, Mogens; Juhas, Pavol
  • Journal of the American Chemical Society, Vol. 134, Issue 15
  • DOI: 10.1021/ja300978f

The kinetics of precipitation from supersaturated solid solutions
journal, April 1961

Number of relevant independent points in x-ray-absorption fine-structure spectra
journal, October 1993

Nyquist-Shannon sampling theorem applied to refinements of the atomic pair distribution function
journal, October 2011

Experimental setup for in situ X-ray SAXS/WAXS/PDF studies of the formation and growth of nanoparticles in near- and supercritical fluids
journal, May 2010

  • Becker, Jacob; Bremholm, Martin; Tyrsted, Christoffer
  • Journal of Applied Crystallography, Vol. 43, Issue 4
  • DOI: 10.1107/S0021889810014688

Structure, Size, and Morphology Control of Nanocrystalline Lithium Cobalt Oxide
journal, March 2011

  • Jensen, Kirsten M. Ø.; Christensen, Mogens; Tyrsted, Christoffer
  • Crystal Growth & Design, Vol. 11, Issue 3
  • DOI: 10.1021/cg101271d

In Situ High-Energy Synchrotron Radiation Study of Boehmite Formation, Growth, and Phase Transformation to Alumina in Sub- and Supercritical Water
journal, October 2009

  • Lock, Nina; Bremholm, Martin; Christensen, Mogens
  • Chemistry - A European Journal, Vol. 15, Issue 48
  • DOI: 10.1002/chem.200901269

Determining Quantitative Kinetics and the Structural Mechanism for Particle Growth in Porous Templates
journal, October 2011

  • Zhao, Haiyan; Nenoff, Tina M.; Jennings, Guy
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 21
  • DOI: 10.1021/jz201260n

Crystal growth by oriented attachment: kinetic models and control factors
journal, January 2014

  • Xue, Xiaogang; Penn, R. Lee; Leite, Edson Roberto
  • CrystEngComm, Vol. 16, Issue 8
  • DOI: 10.1039/c3ce42129e

Neutron Total Scattering Analysis of Nanoparticles
journal, January 2012

Watching Nanoparticles Form: An In Situ (Small-/Wide-Angle X-ray Scattering/Total Scattering) Study of the Growth of Yttria-Stabilised Zirconia in Supercritical Fluids
journal, March 2012

  • Tyrsted, Christoffer; Pauw, Brian Richard; Jensen, Kirsten Marie Ørnsbjerg
  • Chemistry - A European Journal, Vol. 18, Issue 18
  • DOI: 10.1002/chem.201102826

In situ Study of the Crystallization from Amorphous to Cubic Zirconium Oxide:  Rietveld and Reverse Monte Carlo Analyses
journal, June 2007

  • Zhang, Feng; Chupas, Peter J.; Lui, Siu Lun Alan
  • Chemistry of Materials, Vol. 19, Issue 13
  • DOI: 10.1021/cm061739w

PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals
journal, July 2007

In-Situ Monitoring of the Formation of Crystalline Solids
journal, February 2011

  • Pienack, Nicole; Bensch, Wolfgang
  • Angewandte Chemie International Edition, Vol. 50, Issue 9
  • DOI: 10.1002/anie.201001180

Understanding the Formation and Evolution of Ceria Nanoparticles Under Hydrothermal Conditions
journal, August 2012

  • Tyrsted, Christoffer; Ørnsbjerg Jensen, Kirsten Marie; Bøjesen, Espen Drath
  • Angewandte Chemie International Edition, Vol. 51, Issue 36
  • DOI: 10.1002/anie.201204747

Subcritical solvothermal synthesis of condensed inorganic materials
journal, June 2002

  • Walton, Richard I.
  • Chemical Society Reviews, Vol. 31, Issue 4
  • DOI: 10.1039/b105762f

Nanostructured materials for advanced energy conversion and storage devices
journal, May 2005

  • Aricò, Antonino Salvatore; Bruce, Peter; Scrosati, Bruno
  • Nature Materials, Vol. 4, Issue 5, p. 366-377
  • DOI: 10.1038/nmat1368

Reactions at supercritical conditions: Applications and fundamentals
journal, July 1995

  • Savage, Phillip E.; Gopalan, Sudhama; Mizan, Thamid I.
  • AIChE Journal, Vol. 41, Issue 7
  • DOI: 10.1002/aic.690410712

Kinetics of Phase Change. II Transformation‐Time Relations for Random Distribution of Nuclei
journal, February 1940

  • Avrami, Melvin
  • The Journal of Chemical Physics, Vol. 8, Issue 2
  • DOI: 10.1063/1.1750631

Granulation, Phase Change, and Microstructure Kinetics of Phase Change. III
journal, February 1941

  • Avrami, Melvin
  • The Journal of Chemical Physics, Vol. 9, Issue 2, p. 177-184
  • DOI: 10.1063/1.1750872

In-situ Synchrotron X-ray Diffraction Study of the Formation of Cubic Li2TiO3 Under Hydrothermal Conditions
journal, March 2011

  • Laumann, Andreas; Ørnsbjerg Jensen, Kirsten Marie; Tyrsted, Christoffer
  • European Journal of Inorganic Chemistry, Vol. 2011, Issue 14
  • DOI: 10.1002/ejic.201001133

Time-Resolved in Situ Neutron Diffraction under Supercritical Hydrothermal Conditions: A Study of the Synthesis of KTiOPO 4
journal, October 2012

  • Ok, Kang Min; Lee, Dong Woo; Smith, Ronald I.
  • Journal of the American Chemical Society, Vol. 134, Issue 43
  • DOI: 10.1021/ja3088696

An EXAFS Study of Nanocrystalline Yttrium Stabilized Cubic Zirconia Films and Pure Zirconia Powders
journal, October 2000

  • Rush, Georgina E.; Chadwick, Alan V.; Kosacki, Igor
  • The Journal of Physical Chemistry B, Vol. 104, Issue 41
  • DOI: 10.1021/jp001105r

Review of supercritical fluids in inorganic materials science
journal, September 2006

  • Aymonier, Cyril; Loppinet-Serani, Anne; Reverón, Helen
  • The Journal of Supercritical Fluids, Vol. 38, Issue 2
  • DOI: 10.1016/j.supflu.2006.03.019

Crystal structure determination of Zr(OH)2(NO3)2 · 4.7H2O from X-ray powder diffraction data
journal, September 1991

In-Situ Synchrotron Radiation Study of Formation and Growth of Crystalline Ce x Zr 1− x O 2 Nanoparticles Synthesized in Supercritical Water
journal, March 2010

  • Tyrsted, Christoffer; Becker, Jacob; Hald, Peter
  • Chemistry of Materials, Vol. 22, Issue 5
  • DOI: 10.1021/cm903316s

Electrolytes for solid oxide fuel cells
journal, November 2006

Nucleation Control in the Aggregative Growth of Bismuth Nanocrystals
journal, January 2011

  • Richards, Vernal N.; Shields, Shawn P.; Buhro, William E.
  • Chemistry of Materials, Vol. 23, Issue 2
  • DOI: 10.1021/cm101957k

WinXAS a Program for X-ray Absorption Spectroscopy Data Analysis under MS-Windows
journal, March 1998

Two-dimensional detector software: From real detector to idealised image or two-theta scan
journal, January 1996

  • Hammersley, A. P.; Svensson, S. O.; Hanfland, M.
  • High Pressure Research, Vol. 14, Issue 4-6, p. 235-248
  • DOI: 10.1080/08957959608201408

Watching Nanoparticles Grow:  The Mechanism and Kinetics for the Formation of TiO 2 -Supported Platinum Nanoparticles
journal, November 2007

  • Chupas, Peter J.; Chapman, Karena W.; Jennings, Guy
  • Journal of the American Chemical Society, Vol. 129, Issue 45
  • DOI: 10.1021/ja076437p

ATOMS : crystallography for the X-ray absorption spectroscopist
journal, March 2001

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