LETTERS
nature materials | VOL 3 | DECEMBER 2004 | www.nature.com/naturematerials 891
Ultra-large-scale syntheses of
monodisperse nanocrystals
JONGNAM PARK
1
, KWANGJIN AN
1
, YOSUN HWANG
2
, JE-GEUN PARK
2
, HAN-JIN NOH
3
,
JAE-YOUNG KIM
3
, JAE-HOON PARK
3
, NONG-MOON HWANG
4
AND TAEGHWAN HYEON
1
*
1
National Creative Research Center for Oxide Nanocrystalline Materials and School of Chemical Engineering, Seoul National University, Seoul 151-744, Korea
2
Department of Physics and Institute of Basic Science, Sungkyunkwan University, Suwon 440-746, Korea
3
Department of Physics and Pohang Light Source, Pohang University of Science and Technology, Pohang 790-784, Korea
4
School of Materials Science & Engineering and Nano-Systems Institute (NSI-NCRC), Seoul National University, Seoul 151-744, Korea
*e-mail: thyeon@plaza.snu.ac.kr
Published online: 28 November 2004; doi:10.1038/nmat1251
T
he development of nanocrystals has been intensively pursued,
not only for their fundamental scientifc interest, but also
for many technological applications
1–3
. Te synthesis of
monodisperse nanocrystals (size variation <5%) is of key importance,
because the properties of these nanocrystals depend strongly on their
dimensions. For example, the colour sharpness of semiconductor
nanocrystal-based optical devices is strongly dependent on the
uniformity of the nanocrystals
3–6
, and monodisperse magnetic
nanocrystals are critical for the next-generation multi-terabit
magnetic storage media
7–9
. For these monodisperse nanocrystals
to be used, an economical mass-production method needs to be
developed. Unfortunately, however, in most syntheses reported so
far, only sub-gram quantities of monodisperse nanocrystals were
produced. Uniform-sized nanocrystals of CdSe (refs 10,11) and Au
(refs 12,13) have been produced using colloidal chemical synthetic
procedures. In addition, monodisperse magnetic nanocrystals
such as Fe (refs 14,15), Co (refs 16–18), γ-Fe
2
O
3
(refs 19,20), and
Fe
3
O
4
(refs 21,22) have been synthesized by using various synthetic
methods
23
. Here, we report on the ultra-large-scale synthesis of
monodisperse nanocrystals using inexpensive and non-toxic
metal salts as reactants. We were able to synthesize as much as
40 g of monodisperse nanocrystals in a single reaction, without a
size-sorting process. Moreover, the particle size could be controlled
simply by varying the experimental conditions. Te current
synthetic procedure is very general and nanocrystals of many
transition metal oxides were successfully synthesized using a very
similar procedure.
The process conditions required for the synthesis of monodisperse
particles of micrometre size
24
are relatively well established, and a
similar principle could be applied to the synthesis of uniform-sized
nanocrystals. The inhibition of additional nucleation during growth,
in other words, the complete separation of nucleation and growth,
is critical for the successful synthesis of monodisperse nanocrystals.
Our research group developed new procedures for the synthesis of
monodisperse nanocrystals of metals
19,23,25
, metal oxides
19,26,27
, and
metal sulphides
28
without a laborious size-sorting process. In particular,
during the direct synthesis of monodisperse iron and iron oxide
nanocrystals
19,23
, we were able to ascertain that the iron–oleate complex,
which is generated in situ from the reaction of iron pentacarbonyl and
oleic acid, is decomposed and acts effectively as a growth source in
synthesizing monodisperse nanocrystals with increased particle size.
From these results, we reasoned that a metal–surfactant complex would
make an effective growth source for the synthesis of monodisperse
nanocrystals. The overall synthetic procedure is depicted in Fig. 1 and
the detailed experimental procedures are described in the Methods
section. Instead of using toxic and expensive organometallic
compounds such as iron pentacarbonyl, we prepared the metal–
oleate complex by reacting inexpensive and environmentally friendly
compounds, namely metal chlorides and sodium oleate. The Fourier
transform infrared spectrum of the iron–oleate complex, which was
prepared by reacting iron chloride (FeCl
3
·6H
2
O) and sodium oleate,
shows a C=O stretching peak at 1,700 cm
–1
, which is a characteristic
peak for a metal–oleate complex (see Supplementary Information,
Fig. S1). The iron–oleate complex in 1-octadecene was slowly heated
Metal
chloride
Na–oleate
Metal–oleate
complex
Metal–oleate
complex
+ + NaCl
Thermal decomposition
in high boiling solvent
Monodisperse
nanocrystals
20 nm
Figure 1 The overall scheme for the ultra-large-scale synthesis of
monodisperse nanocrystals. Metal–oleate precursors were prepared from the
reaction of metal chlorides and sodium oleate. The thermal decomposition of the
metal–oleate precursors in high boiling solvent produced monodisperse nanocrystals.
©2004 Nature Publishing Group