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Methods of synthesizing ruthenium and osmium compounds

A technology of compounds and ruthenium complexes, applied in the directions of osmium organic compounds, ruthenium organic compounds, phosphorus organic compounds, etc., can solve problems such as long reaction time, no teaching or suggestion of reaction route, etc.

Inactive Publication Date: 2007-01-10
PRAXAIR TECH INC
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0008] Although the scheme of prior art adopts non-reactive solvent system to synthesize formula L x M(CO) y [L = neutral ligand, M = Ru or Os, x = 1-4, and y = 1-5] compound, but does not teach or suggest a neat or solvent-free reaction route
Furthermore, prior art references indicate that the synthesis of carbonyl-based complexes, i.e. ruthenium complexes, requires long reaction times

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0019] Preferred embodiments of the invention are described herein.

[0020] Will Ru 3 (CO) 12(2.0 g, 3.13 mMol) was transferred to a dry 25 ml round bottom flask equipped with a water condenser and a Teflon-coated magnetic stir bar. 1,3-Cyclohexadiene (5 ml, 52.5 mMol, greater than 5-fold excess) was added using a syringe. Under a dry nitrogen atmosphere, the mixture was heated to reflux with stirring for 5 hours to obtain a clear yellow solution. Heating was stopped to allow the mixture to cool to room temperature. Excess 1,3-cyclohexadiene was removed using rotary evaporation. Under the pressure of 0.1 torr, carry out vacuum distillation to obtain 1,3-cyclohexadienetricarbonyl ruthenium (C 6 h 8 )Ru(CO) 3 (2.1 g, 7.92 mMol, 84% yield).

[0021] Using GC-MS, 1 H NMR, 13 C NMR, FTIR, and ICP-MS (metal content) to characterize the compound. The obtained analysis data ( 1 H& 13 C NMR) consistent with literature values ​​for this compound. Figures 1, 2 and 3 show t...

Embodiment 2

[0023] This is another example where it is expected that triosmium dodecacarbonyl (Os 3 CO 12 ) and 1,3-cyclohexadiene generate 1,3-cyclohexadiene tricarbonyl osmium (C 6 h 8 )Os(CO) 3 . This reaction was carried out under the same conditions as in Example 1 above. 2gOs 3 (CO) 12 (2.2mMol) into the flask. Then about 5 ml of 1,3-cyclohexadiene (52.5 mMol, >5-fold excess) was added and the mixture was refluxed for several hours. The substitution of osmium for ruthenium proceeded in similar yields, physical properties and reactivity. This is consistent with the generally accepted periodic nature of the elements.

[0024] The present invention's most preferred preparation process step of ruthenium and osmium compound is as follows:

Embodiment 3

[0026] 87.26g (0.136Mol) Ru 3 (CO) 12 Place into a 3-neck RB flask equipped with a Teflon-coated magnetic stir bar, condenser, and gas stopcock. Add 220ml (185g, 2.31mol) C 6 h 8 . The device was flushed with nitrogen and then kept under nitrogen for the remainder of the process. The mixture was heated to gentle reflux and stirred for 44 hours, at which point it was a cloudy yellow / orange mixture. At 80 °C, under atmospheric pressure, the mixture yielded 120 ml of unreacted C 6 h 8 . Vacuum distillation (at P = 0.1 Torr) of the remaining mixture yielded 103.32 g (C 6 h 8 )Ru(CO) 3 (0.39 mol, 95% yield) (>99.8% by GC-MS).

[0027] Excess ligand was removed by distillation. The refluxed reaction mixture was subjected to rotary evaporation at ≈10 Torr and 60 °C, due to the 1,3-C 6 h 8 A lower relative vapor pressure, such that removal of excess of the species removes non-reactive solvent and excess ligand. Finally, the resulting refluxed reaction mixture from which...

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PUM

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Abstract

This invention is directed to a method for synthesizing a carbonyl based compound under neat conditions comprising refluxing a metal carbonyl compound with an excess of neutral ligand to produce a first mixture; evaporating any excess neutral ligand from the first mixture to produce a second mixture; and distilling the second mixture to produce the carbonyl based compound.

Description

field of invention [0001] The invention relates to a method for synthesizing organometallic materials. More specifically, the present invention relates to methods for the synthesis of ruthenium and osmium compounds. Background of the invention [0002] Ruthenium (Ru), osmium (Os), and their oxides are materials expected to be used as electrodes in future semiconductor devices such as ferroelectric memories and logic chips. These materials exhibit attractive physical properties such as low electrical resistance, high work function, resistance to interlayer chemical diffusion, and thermal and oxidative stability. In addition, ruthenium, osmium, and their oxides produce thin films with lattice parameters and thermal expansion coefficients that make them compatible with many dielectric materials expected to be used in future semiconductor devices. [0003] Chemical Vapor Deposition (CVD) is a technique widely used in the manufacture of semiconductor devices to produce the laye...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C07F9/02C07F15/00C23C16/00C07C13/23
CPCC07F15/0046C07F15/002C07F15/00
Inventor M·A·里恩哈德C·A·胡维
Owner PRAXAIR TECH INC