Acta Cryst. (1992). B48, 747-752
From Crystal Structure Data Towards Reaction Paths in the Solid State?
BY A. VEGAS AND M. MARTiNEZ-RIPOLL
UEI de Cristalograf[a, Instituto Rocasolano, CSIC, Serrano 119, E-28006 Madrid, Spain
(Received 17 January 1992; accepted 15 April 1992)
747
Abstract
The structures of FeB, GdSi, Re3B, Ni2In and
6-Ni2Si are analyzed on the basis of their parent
metal structures which become modified during com-
pound formation. The observed metallic fragments
maintain the original topology and distances, and the
small distortions observed in them do not occur
randomly, but are correlated as in molecular com-
pounds. This analysis is not only used to describe the
structures in a simpler way, but also to infer plausi-
ble reaction mechanisms in the solid state.
Introduction
Metal clusters have been widely studied and much of
the work, aimed at correlating physical properties
with structural and bonding aspects, has been col-
lected in reviews (Franzen, 1978; Jansen, 1987;
Simon, 1981, 1988; Hughbanks, 1989).
Until recently, the existence of metal clusters was
seen as a logical feature in interstitial compounds,
which were considered as bulky metals, slightly dis-
torted by the inclusion of small amounts of other
atoms (see Wells, 1975). This was also true of the
so-called metal-rich compounds, in which the
unsaturated valences of the metal atoms are used to
form metal-metal bonds. As examples of the latter
we may mention Fe3C (Lipson & Petch, 1940) and
Cs~O3 (Simon, 1988), both clearly related to Fe and
Cs metals, respectively.
These bonding aspects led Franzen (1978) to con-
sider the metal-rich compounds as modified metals in
which the metallic interactions are partially modified
as the result of metal-nonmetal bonding. Other
examples of relating the metal substructure to the
parent metal can be found in the articles of Simon
(1981, 1988), dealing with structure and bonding in
clusters of metal-rich compounds and clusters of
valence-electron-poor metals. More explicit referen-
ces to such a relationship can be found in the articles
dealing with d ~° metal aggregates (see Jansen, 1987)
and in an article devoted to the bonding in clusters
and condensed clusters of early transition and rare-
earth metals (Hughbanks, 1989).
However, in an independent way, and looking for
an alternative to the model of O'Keeffe & Hyde
0108-7681/92/060747-06506.00
(1981, 1985) for describing crystal structures, we
have shown that the relationship between the struc-
ture of the parent metal and the metal substructure
in a given compound is not restricted to compounds
with unsaturated bonding. It also appears in com-
pounds with saturated valences [apatite:
Cas(POa)3(OH,F), olivine: Mg2SiO4, etc], even in
compounds traditionally considered as ionic (KC103)
or those such as TiO2, which is far from being
considered a metal-rich compound (Vegas, Romero
& Martinez-Ripoll, 1990, 1991). For some of the
structures discussed there, a possible reaction
mechanism was advanced in the sense that metallic
fragments observed in many structures could be seen
to be the result of a process of either dynamic
deformation or breaking up, initiated in the parent
metal.
In the present work we apply this model to simple
binary compounds such as FeB, GdSi, Re3B, Ni2In
and &-Ni2Si in order to deduce a plausible reaction
path from the examination of the metallic fragments
appearing in them.
Discussion
The FeB structure and elemental Fe
Iron presents the phases collected in Table 1
(Landolt-B/brnstein, 1971). The FeB structure
(Hendricks & Kosting, 1930) is orthorhombic, Pnma,
with a = 5.495, b = 2.946 and c = 4.053 ~, and is
represented in Fig. l(a). The classical description
consists of columns of face-sharing Fe6 trigonal
prisms running parallel to the b axis. The columns
are linked by additional edge-sharing. The B atoms
are off-center of these trigonal prisms. Parth+ (1981)
has described the structure as a twinned h.c.p.
arrangement of Fe atoms with boron in the trigonal
prisms generated at the twin plane. O'Keeffe & Hyde
(1985) have related this structure to the cation arrays
of many sulfates, selenates, chromates, etc.
Our alternative description is based on the space
between trigonal prisms (shaded in Fig. l a). These
apparently empty holes are really fragments of a
body centered cubic net, the Fe---Fe distances being
within a few percent of those of the high-temperature
b.c.c, phase of metallic iron. The fragments are easily
© 1992 International Union of Crystallography