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In-Situ Synchrotron Radiation Study of Formation and Growth of Crystalline CexZr1-xO2 Nanoparticles Synthesized in Supercritical Water

Tyrsted, Christoffer; Becker, Jacob; Hald, Peter; Bremholm, Martin; Pedersen, Jan Skov; Chevallier, Jacques; Cerenius, Yngve LU ; Iversen, Steen B. and Iversen, Bo B. (2010) In Chemistry of Materials 22(5). p.1814-1820
Abstract
In situ synchrotron powder X-ray diffraction (PXRD) measurements have been conducted to follow the nucleation and growth of crystalline CexZr1-xO2 nanoparticles synthesized in supercritical water with a full substitution variation (x = 0, 0.2, 0.5, 0.8, and 1.0). Direction-dependent growth curves are determined and described using reaction kinetic models. A disctinct change in growth kinetics is observed with increasing cerium content. For x = 0.8 and 1.0 (high cerium content), the growth in initially limited by the surface reaction kinetics, however, at a size of similar to 6 nm, the growth changes and becomes limited by the diffusion of monomers toward the surface. For x = 0 and 0.2, the opposite behavior is observed with the growth... (More)
In situ synchrotron powder X-ray diffraction (PXRD) measurements have been conducted to follow the nucleation and growth of crystalline CexZr1-xO2 nanoparticles synthesized in supercritical water with a full substitution variation (x = 0, 0.2, 0.5, 0.8, and 1.0). Direction-dependent growth curves are determined and described using reaction kinetic models. A disctinct change in growth kinetics is observed with increasing cerium content. For x = 0.8 and 1.0 (high cerium content), the growth in initially limited by the surface reaction kinetics, however, at a size of similar to 6 nm, the growth changes and becomes limited by the diffusion of monomers toward the surface. For x = 0 and 0.2, the opposite behavior is observed with the growth initially being limited by diffusion (up to similar to 3.5 nm) and later by the surface reaction kinetics. Thus, although a continuous solid solution can be obtained for the ceria-zirconia system, the growth of ceria and zirconia nanoparticles is fundamentally different under supercritical flow reactor. The resulting samples were analyzed using PXRD, small-angle X-ray scattering (SAXS), and transmission electron microscopy (TEM). The nanoparticles with x = 0, 0.2, and 0.5 have very low polydispersities. The sizes range from 4 nm to 7 nm, and the particles exhibit a reversibly pH-dependent agglomeration. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Chemistry of Materials
volume
22
issue
5
pages
1814 - 1820
publisher
The American Chemical Society
external identifiers
  • wos:000274929000028
  • scopus:77949343598
ISSN
0897-4756
DOI
10.1021/cm903316s
language
English
LU publication?
yes
id
a5446d58-a901-49bb-a616-e50bac1a0e42 (old id 1568287)
date added to LUP
2010-03-23 14:33:24
date last changed
2018-05-29 10:14:29
@article{a5446d58-a901-49bb-a616-e50bac1a0e42,
  abstract     = {In situ synchrotron powder X-ray diffraction (PXRD) measurements have been conducted to follow the nucleation and growth of crystalline CexZr1-xO2 nanoparticles synthesized in supercritical water with a full substitution variation (x = 0, 0.2, 0.5, 0.8, and 1.0). Direction-dependent growth curves are determined and described using reaction kinetic models. A disctinct change in growth kinetics is observed with increasing cerium content. For x = 0.8 and 1.0 (high cerium content), the growth in initially limited by the surface reaction kinetics, however, at a size of similar to 6 nm, the growth changes and becomes limited by the diffusion of monomers toward the surface. For x = 0 and 0.2, the opposite behavior is observed with the growth initially being limited by diffusion (up to similar to 3.5 nm) and later by the surface reaction kinetics. Thus, although a continuous solid solution can be obtained for the ceria-zirconia system, the growth of ceria and zirconia nanoparticles is fundamentally different under supercritical flow reactor. The resulting samples were analyzed using PXRD, small-angle X-ray scattering (SAXS), and transmission electron microscopy (TEM). The nanoparticles with x = 0, 0.2, and 0.5 have very low polydispersities. The sizes range from 4 nm to 7 nm, and the particles exhibit a reversibly pH-dependent agglomeration.},
  author       = {Tyrsted, Christoffer and Becker, Jacob and Hald, Peter and Bremholm, Martin and Pedersen, Jan Skov and Chevallier, Jacques and Cerenius, Yngve and Iversen, Steen B. and Iversen, Bo B.},
  issn         = {0897-4756},
  language     = {eng},
  number       = {5},
  pages        = {1814--1820},
  publisher    = {The American Chemical Society},
  series       = {Chemistry of Materials},
  title        = {In-Situ Synchrotron Radiation Study of Formation and Growth of Crystalline CexZr1-xO2 Nanoparticles Synthesized in Supercritical Water},
  url          = {http://dx.doi.org/10.1021/cm903316s},
  volume       = {22},
  year         = {2010},
}