Bifunctional Chalcogen Linkers for the Stepwise Generation of Multimetallic Assemblies and Functionalized Nanoparticles
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资源简介：
The disulfide ligand
(SC6H4CO2H-4)2 acts as
a simple but versatile linker for a range of group 8 transition metals
through reaction of the oxygen donors. This leads to a range of homobimetallic
ruthenium and osmium alkenyl compounds, [{M(CHCHR)(CO)(PPh3)2(O2CC6H4S-4)}2] (M = Ru, Os; R = C6H4Me-4). Additional
metal-based functionality can be added through the use of precursors
incorporating rhenium bipyridine units (R = (bpy)ReCl(CO)3). The more robust diphosphine ligands in [{Ru(dppm)2(O2CC6H4S-4)}2]2+ (dppm = diphenylphosphinomethane) allow reduction of the disulfide
bond with sodium borohydride to yield the thiol complex [Ru(O2CC6H4SH-4)(dppm)2]+. This complex reacts with [AuCl(PPh3)] to afford the
bimetallic compound [Ru(dppm)2(O2CC6H4S-4)Au(PPh3)]+. However, an improved
route to the same and related heterobimetallic compounds is provided
by the reaction of cis-[RuCl2(dppm)2] with [Au(SC6H4CO2H-4)(L)]
(L = PPh3, PCy3, PMe3, IDip) in the
presence of base and NH4PF6 (IDip = 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidene).
The heterotrimetallic compound [Au(SC6H4CO2Ru(dppm)2)2]+ is accessible
through the reaction of the homoleptic gold(I) dithiolate [Au(SC6H4CO2H-4)2]PPN (PPN = bis(triphenylphosphine)iminium)
with cis-[RuCl2(dppm)2]. Without
departure from the same methodology, greater complexity can be incorporated
into the system to provide the penta- and heptametallic assemblies
[(dppf){AuSC6H4CO2Ru(dppm)2}2]2+ and [(dppf){AuSC6H4CO2Os(CHCH-bpyReCl(CO)3)(CO)(PPh3)2}2]. The same stepwise approach provides
the dinuclear organometallic complexes [(L)Au(SC6H4CO2-4)M(CHCHC6H4Me-4)(CO)(PPh3)2] (M = Ru, Os; L = PPh3, IDip). Complexes
containing three metals from different groups of the periodic table
[(L)Au(SC6H4CO2-4)M{CHCH-bpyReCl(CO)3}(CO)(PPh3)2] (M = Ru, Os) can also
be prepared, with one ruthenium example (L = PPh3) being
structurally characterized. In order to illustrate the versatility
of this approach, the synthesis and characterization (IR and NMR spectroscopy,
TEM, EDS, and TGA) of the functionalized gold and palladium nanoparticles
Au@[SC6H4CO2Ru(dppm)2]+ and Pd@[SC6H4CO2Ru(dppm)2]+ is reported.
创建时间：
2016-12-05
