ELSEVIER Inorganica Chimica Acta 230 (1995) 219-223
Synthesis of polymer-
complexes
Note
and silica-supported manganese phosphine
and their reaction with oxygen
Guang Qing Li, Rakesh Govind *
Department of Chemical Engineering, University of Cincinnati, Cincinnati, OH 45221, USA
Received 3 May 1994; revised 20 July 1994
Abstract
A series of polymer- and silica-supported manganese phosphine complexes has been prepared and characterized. These
complexes react reversibly with molecular oxygen in the solid state to yield 1:1 Mn:O2 adducts. The reaction may be reversed
either by a pressure drop or a temperature rise. All the 02 adducts are highly colored and binding curves as a function of
the partial pressure of oxygen have been constructed. The silica-supported complexes can be prepared from ligand-silanes
either by reaction with dehydrated silica and then with anhydrous manganese(II) bromide or vice versa.
Keywords: Manganese complexes; Phosphine complexes; Dioxygen complexes; Silica-supported complexes; Polymeric complexes
1. Introduction
Many highly active and selective catalysts can be
derived from transition metal complexes and the prop-
crties of these catalysts may often be varied widely by
a change in the electronic and steric environment of
the metal center. However, these homogeneous catalysts
are often more difficult to handle than heterogeneous
catalysts. On an industrial scale, problems associated
with homogeneous catalysts include corrosion, depo-
sition of the catalyst on the wall of the reactor and
expensive recovery of the catalyst from the reaction
products. One way of overcoming these problems while
retaining the advantages of the transition metal complex
catalysts is to anchor homogeneous catalysts to polymers
or other supports effectively 'heterogenizing' them, and
this technique is currently attracting widespread interest
[1].
In recent years there has been a rapid growth in
the use of supporting transition metal complexes mainly
as catalysts for hydrogenation, hydroformylation, hy-
drosilylation and isomerization reactions [2]. Apart from
the obvious advantage of ease of recovery, the thermal
stabilities of such complexes are frequently higher than
those of their homogeneous counterparts and they are
often less sensitive to oxidation and moisture.
* Corresponding author.
Our interest in manganese(II) tertiary phosphine
complexes stems from the fact that they are able
reversibly to bind dioxygen and other small molecules
either in the solid state or in solution [3,4]. This
reversibility of the 02 binding appears to have potential
as a practical means as an oxidation catalyst and as
an absorbent for removing oxygen from air. In an effort
to improve the chemical robustness of the complexes
we have synthesized a number of polymer- and silica-
supported manganese phosphine complexes.
2. Results and discussion
The ligand-polymers were synthesized by the reaction
of LiPR2 (R = Me, Ph) with the corresponding polyvinyl
chloride (PVC) and poly-p-bromostyrene (PBS). Ele-
mental analyses of the products indicated that the
reactions proceeded nearly to completion with typically
only a small amount of residual chlorine or bromine
( < 0.1%) remaining on the polymer. The phosphinated
polymers were then reacted with the manganese(II)
salts, MnX2 (X=C1, Br or I), in a 1:1 molar ratio in
anhydrous solvent in an inert atmosphere to give the
supported complexes (Scheme 1 and Table 1).
Liganding groups can be chemically bonded to the
surface of macromolecules. Thus transition metal com-
plexes may be prepared which are highly dispersed on
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