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energy was found to be 51.9 kJ/mol and a Langmuir – Hinshelwood rate expression was used to represent the data. It was found that growth rate was zero order with respect to pressure, precursor concentration and hydrogen concentration. However, at low concentrations of either precursor or hydrogen, half order dependence was noted. All byproducts studied indicated a negative effect on growth rate as concentration was increased. It was proposed that the rate determining step was the surface reaction. The deposition of ruthenium from Ru(tmhd)2cod, although analogous in process to the deposition of copper from Cu(tmod)2, is much more complicated mechanistically due to the addition of a cyclooctadiene ligand and its behavior in SCCO2. Cod has been shown to enhance solubility of precursors in SCCO2 because it can shield the positive electrical charge of various metal centers.47 However, as the reaction proceeds and the cod concentration increases, a negative effect on growth rate is observed due to its competition for hydrogen in order to reduce to its monoene and its competition for surface active sites, thereby reducing the number of available sites to allow the desired reaction to continue. A number of studies have been carried out in order to better understand the hydrogenation of cod. It was observed that 1,5 cod is isomerized to the conjugated diene, 1,3 cod, due to the lower energy state.57 The conjugated diene then more quickly hydrogenated to coe. Additionally, the presence of cod and its ability to more readily adsorb to the surface hindered the following hydrogenation of coe to cot. It was found that the activation energy for the reduction of cod to coe over a Pd/α-Al2O3 catalyst was 74 kJ/mol while the activation energy was 98 kJ/mol for coe to cot.58 Haas and Gaube59 reported that the hydrogenation of cod occurs 6 times faster than the hydrogenation of 45PDF Image | Supercritical Fluid Deposition Of Thin Metal Films
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