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The Gibbs free energy of the equilibrium reaction was estimated at-2.1 kcal mol-1 (at 298.15 K and 1 atm) using model compounds, where methyl groups of Cp*were replaced by hydrogen atoms; this supports the fact that
-
The Gibbs free energy of the equilibrium reaction was estimated at-2.1 kcal mol-1 (at 298.15 K and 1 atm) using model compounds, where methyl groups of Cp*were replaced by hydrogen atoms; this supports the fact that 4 was more basic than 3.
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note
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Density functional theory (DFT) calculations were carried out at the B3PW91 level in conjunction with the Stuttgart/Dresden ECP19 and associated with triple-^ SDD basis sets for Ru and Os. For H and C, 6-311G(d,p) and 6-31G(d) basis sets, respectively, were employed. The Ru3 core in 1 was almost an equilateral triangle with sides of av 2.7497 A and contained three doubly bridging and two triply bridging hydrido ligands.2a To confirm that the above-mentioned basis sets were able to reproduce the geometries of the pentahydride, the geometry of (CpRu)3(u-H)2(u-H)3 (1a), whose factual structure was accurately characterized by X-ray diffraction studies, was optimized. The optimized geometry shown in Figure S1 corresponds well with crystal structures, and the average Ru- Ru distance of 1a is 2.7348 A; this average varies within 0.015 A between theory and experiments (details are provided in the Supporting Information). Therefore, we employed the basis sets and optimized the geometries of 3 and 4.
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The systems, 0.8x + 0.2y = 2.700 (1) and 0.4x + 0.6y = 2.747 (2), should be solved for 3', where d(Ru-(H)2-Os) = x and d(Os-H-Os) = y.
-
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