Thomas J O'Hare

US Patent:

49924800, Feb 12, 1991

Filed:

Mar 29, 1990

Appl. No.:

7/500935

Inventors:

Devinder Mahajan - Port Jefferson NY
Richard S. Sapienza - Shoreham NY
William A. Slegeir - Hampton Bays NY
Thomas E. O'Hare - Huntington Station NY

Assignee:

Associated Universities, Inc. - Washington DC

International Classification:

C07C 2706

US Classification:

518700

Abstract:

There is disclosed synthesis of CH. sub. 3 OH from carbon monoxide and hydrogen using an extremely active homogeneous catalyst for methanol synthesis directly from synthesis gas. The catalyst operates preferably between 100. degree. -150. degree. C. and preferably at 100-150 psia synthesis gas to produce methanol. Use can be made of syngas mixtures which contain considerable quantities of other gases, such as nitrogen, methane or excess hydrogen. The catalyst is composed of two components: (a) a transition metal carbonyl complex and (b) an alkoxide component. In the simplest formulation, component (a) is a complex of nickel tetracarbonyl and component (b) is methoxide (CH. sub. 3 O. sup. -), both being dissolved in a methanol solvent system. The presence of a co-solvent such as p-dioxane, THF, polyalcohols, ethers, hydrocarbons, and crown ethers accelerates the methanol synthesis reaction.

US Patent:

46199462, Oct 28, 1986

Filed:

Dec 23, 1985

Appl. No.:

6/812705

Inventors:

Richard S. Sapienza - Shoreham NY
William A. Slegeir - Hampton Bays NY
Thomas E. O'Hare - Huntington Station NY
Devinder Mahajan - Selden NY

International Classification:

C07C 2706
C07C 3104

US Classification:

518700

Abstract:

A catalyst and process useful at low temperatures (below about 160. degree. C. ) and preferably in the range 80. degree. -120. degree. C. used in the production of methanol from carbon monoxide and hydrogen is disclosed. The catalyst is used in slurry form and comprises a complex reducing agent derived from the component structure NaH--RONa--M(OAc). sub. 2 where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1-6 carbon atoms. This catalyst is preferably used alone but is also effective in combination with a metal carbonyl of a group VI (Mo, Cr, W) metal. The preferred catalyst precursor is Nic (where M=Ni and R=tertiary amyl). Mo(CO). sub. 6 is the preferred metal carbonyl if such component is used. The catalyst is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.

US Patent:

49353950, Jun 19, 1990

Filed:

Jan 7, 1988

Appl. No.:

7/141454

Inventors:

Devinder Mahajan - Port Jefferson NY
Richard S. Sapienza - Shoreham NY
William A. Slegeir - Hampton Bays NY
Thomas E. O'Hare - Huntington Station NY

Assignee:

Associated Universities, Inc. - Washington DC

International Classification:

G01J 3120

US Classification:

502 62

Abstract:

There is disclosed synthesis of CH. sub. 3 OH from carbon monoxide and hydrogen using an extremely active homogeneous catalyst for methanol synthesis directly from synthesis gas. The catalyst operates preferably between 100. degree. -150. degree. C. and preferably at 100-150 psia synthesis gas to produce methanol. Use can be made of syngas mixtures which contain considerable quantities of other gases, such as nitrogen, methane or excess hydrogen. The catalyst is composed of two components: (a) a transition metal carbonyl complex and (b) an alkoxide component. In the simplest formulation, component (a) is a complex of nickel tetracarbonyl and component (b) is methoxide (CH. sub. 3 O. sup. 13 ), both being dissolved in a methanol solvent system. The presence of a co-solvent such as p-dioxane, THF, polyalcohols, ethers, hydrocarbons, and crown ethers accelerates the methanol synthesis reaction.

US Patent:

46136231, Sep 23, 1986

Filed:

Jul 23, 1985

Appl. No.:

6/757981

Inventors:

Devinder Mahajan - Selden NY
William A. Slegeir - Hampton Bays NY
Richard S. Sapienza - Shoreham NY
Thomas E. O'Hare - Huntington Station NY

Assignee:

The United States of America as represented by the United States
Department of Energy - Washington DC

International Classification:

C07C 2706

US Classification:

518700

Abstract:

A gas reaction process for the preferential production of methyl formate over the co-production of methanol wherein the reactant ratio of CO/H. sub. 2 is upgraded and this reaction takes place at low temperatures of 50. degree. -150. degree. C. and moderate pressures of. gtoreq. 100 psi.

US Patent:

46147497, Sep 30, 1986

Filed:

Dec 23, 1985

Appl. No.:

6/812707

Inventors:

Richard S. Sapienza - Shoreham NY
William A. Slegeir - Hampton Bays NY
Thomas E. O'Hare - Huntington Station NY
Devinder Mahajan - Selden NY

International Classification:

C07C 2706
C07C 3104

US Classification:

518700

Abstract:

A catalyst and process useful at low temperatures (below about 160. degree. C. ) and preferably in the range 80. degree. -120. degree. C. used in the production of methanol from carbon monoxide and hydrogen is disclosed. The catalyst is used in slurry form and comprises a complex reducing agent derived from the component structure NaH--RONa--M(OAc). sub. 2 where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1-6 carbon atoms. This catalyst is preferably used alone but is also effective in combination with a metal carbonyl of a group VI (Mo, Cr, W) metal. The preferred catalyst precursor is Nic (where M=Ni and R=tertiary amyl). Mo(CO). sub. 6 is the preferred metal carbonyl if such component is used. The catalyst is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.

US Patent:

46236341, Nov 18, 1986

Filed:

Dec 23, 1985

Appl. No.:

6/812708

Inventors:

Richard S. Sapienza - Shoreham NY
William A. Slegeir - Hampton Bays NY
Thomas E. O'Hare - Huntington Station NY
Devinder Mahajan - Selden NY

International Classification:

B01J 3112

US Classification:

502113

Abstract:

A catalyst and process useful at low temperatures (below about 160. degree. C. ) and preferably in the range 80. degree. -120. degree. C. used in the production of methanol from carbon monoxide and hydrogen is disclosed. The catalyst is used in slurry form and comprises a complex reducing agent derived from the component structure NaH--RONa--M(OAc). sub. 2 where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1-6 carbon atoms. This catalyst is preferably used alone but is also effective in combination with a metal carbonyl of a group VI (Mo, Cr, W) metal. The preferred catalyst precursor is Nic (where M=Ni and R=tertiary amyl). Mo(CO). sub. 6 is the preferred metal carbonyl if such component is used. The catalyst is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.