skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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) (SC-22)
OSTI Identifier:
1335051
Grant/Contract Number:  
SC0001085
Resource Type:
Journal Article: 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.
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. doi:10.1107/S2052252514006538.
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. doi:10.1107/S2052252514006538.
@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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1107/S2052252514006538

Citation Metrics:
Cited by: 18 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

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


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

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

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

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