Nanosized copper catalyst precursors for the direct synthesis of trialkoxysilanes
View Patent ↗The present invention provides a process for using nanosized copper, nanosized copper oxides, nanosized copper chlorides, other nanosized copper salts, and mixtures thereof, as sources of catalytic copper in the Direct Synthesis of trialkoxysilanes of the formula HSi(OR) 3 wherein R is an alkyl group containing from 1 to 6 carbon atoms inclusive. The nanosized copper, nanosized copper oxides, nanosized copper chlorides, other nanosized copper salts, and their mixtures of this invention have average particle sizes that are in the range from about 0.1 to about 600 nanometers, preferably from about 0.1 to about 500 nanometers, and most preferably from about 0.1 to about 100 nanometers. Nanosized sources of catalytic copper afford high dispersion of catalytic sites on silicon and contribute to high reaction rates, high selectivity and high silicon conversion. The nanosized copper catalyst precursors of the invention permit the use of substantially reduced levels of copper compared to conventional practice.
1. A process for the direct synthesis of trialkoxysilanes comprising the steps of:
(a) providing a slurry of silicon metal, and a copper catalyst precursor having an average particle size of about 0.1 to 60 nanometers in a thermally stable solvent;
(b) forming a copper-silicon intermetallic;
(c) reacting said copper-silicon intermetallic with an alcohol of formula ROH wherein R is an alkyl group having 1 to 6 carbon atoms inclusive, to form a trialkoxysilane of the formula HSi(OR) 3 wherein R is as previously defined;
(d) recovering the trialkoxysilane; and
(e) remediating the thermally stable solvent for subsequent Direct Synthesis of trialkoxysilanes.
2. The process of claim 1 wherein in step (a) said slurry is formed with nanosized silicon metal.
3. The process of claim 1 wherein in step (a) said silicon metal is produced by acid leaching and said copper catalyst precursor comprises nanosized copper chloride.
4. The process of claim 1 wherein in step (a), said thermally stable solvent is a member selected from the group consisting of linear and branched paraffins, cycloparaffins, alkylated benzenes, aromatic ethers, and polyaromatic hydrocarbons.
5. The process of claim 1 wherein in step (a), an initial copper concentration is about 300 to about 5000 ppm based on an amount of said silicon metal.
6. The process of claim 1 wherein in step (a), said copper catalyst precursor is selected from the group consisting of nanosized copper, nanosized copper oxides, nanosized copper chlorides, other nanosized copper salts, and mixtures thereof.
7. The process of claim 1 wherein in step (b) said copper-silicon intermetallic is formed by heating said copper catalyst precursor in said slurry for about 0.01 to about 24 hours at a temperature of about 20 to about 400° C.
8. The process of claim 1 wherein in step (b) said copper-silicon intermetallic is formed in situ.
9. The process of claim 1 wherein in step (b) said copper-silicon intermetallic is formed in a separate reaction vessel prior to reaction with said alcohol.
10. The process of claim 1 wherein in step (c) said alcohol is introduced as a gaseous stream to react with said copper-silicon intermetallic.
11. The process of claim 1 wherein in step (c) more than one alcohol is present to react with said copper-silicon intermetallic.
12. The process of claim 1 wherein step (c) comprises reacting said copper-silicon intermetallic with ethanol at a temperature of about 200 to about 210° C.