Ultramicroscopy 29 (1989) 233-246 233
North-Holland, Amsterdam
TEM AND IN-SITU EM STUDY OF THE DISPERSION OF MoO 3 ON SiO 2
A. DATTA and J.R. REGALBUTO
Department of Chemical Engineerin~ University of Illinois at Chicago, Chicago, Illinois 60680, USA
and
C.W. ALLEN
Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA
Received at Editorial Office October-November 1988; presented at Conference May 1988
Molybdenum trioxide supported on nonporous silica spheres and planar silica substrates were used with TEM and in-situ
EM (environmental cell and heating stage), respectively, to study the spreading behavior of the hexagonal and orthorhombic
forms of MoO 3 on SiO2. At temperatures below 500 o C, supported orthorhombic crystallites are stable, while supported
hexagonal crystaUites, formed by an initial calcination of the precursor at 300 o C, spread drastically and in doing so produce a
novel, multilayered and amorphous silica-supported morphology for MoO 3. The mechanism of spreading appears to be the
formation of mobile species on hexagonal crystallites, and subsequent migration across the SiO2 surface.
1. Introduction
Supported molybdenum or its trioxide has a
wide variety of uses in heterogeneous catalysis, for
catalytic reactions such as hydrodesulfurization,
hydrogenation and dehydrogenation, reforming,
and hydrocracking, to name a few. The dispersion
and morphology of the trioxide, often a precursor
phase of the final catalyst, have much to do with
final catalytic activity. A number of trioxide forms
exist over various support materials. At low load-
ings, the material is generally completely dispersed
and of a monolayer type while at higher loadings,
bulk crystallites form [1]. Some supports such as
alumina and titania exhibit stronger interactions
with MoO3 such that intermetallic oxide phases
form [2]. Over SiO2, however, only the monolayer
and bulk crystalline (orthorhombic) forms have
been reported; these formed with an initial
calcination of the impregnated precursor always
greater than 450 ° C. At this high initial calcina-
tion temperature, surface loadings less than I atom
Mo/nm 2 [1] yield the well dispersed catalyst,
whose morphology is only slightly altered by sub-
sequent treatments [3], while loadings greater than
this value result in bulk crystallites. There appears
to be no way to redisperse bulk, orthorhombic
crystallites of MoO 3 on SiO3 once they form [4],
short of extremely high calcination temperatures,
at which trioxide losses occur due to volatilization
[5].
In recent characterization of MoO3/SiO 2 cata-
lysts with X-ray diffraction (XRD) among other
methods [6], it has been shown that the dispersion
of high-loading MoO 3 (4 atoms Mo/nm 2) can be
controlled through the initial formation of the
little-studied hexagonal crystalline phase. A
summary of XRD results from this study is shown
in fig. 1. The supported hexagonal phase, formed
by an initial 300 °C air calcination, is shown in
pattern a and is compared to the orthorhombic
phase formed by a 500 °C calcination (pattern b).
A bulk crystalline (poorly dispersed) ortho-
rhombic phase (pattern c) was formed by a 500 ° C
calcination of the poorly dispersed hexagonal
phase, while continued calcination at 300°C
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