Chemical reduction using a catalyst comprising frustrated lewis pairs

Patent metadata

Field	Value
Publication number	US-10329233-B2
Application number	US-201715472009-A
Country	US
Kind code	B2
Filing date	Mar 28, 2017
Priority date	Dec 7, 2012
Publication date	Jun 25, 2019
Grant date	Jun 25, 2019

Abstract

The presently disclosed and/or claimed inventive concept(s) relates generally to the reduction of carbon dioxide by heterogeneous catalysis. More particularly, but not by way of limitation, the presently disclosed and/or claimed inventive concept(s) relates to the reduction of carbon dioxide by heterogeneous catalysis with a heterogeneous hydrogenation catalyst comprising structurally frustrated Lewis pairs, wherein, for example but not by way of limitation, formic acid is produced and hydrocarbons are indirectly produced. In one non-limiting embodiment, the heterogeneous catalyst comprises hexagonal boron nitride (h-BN) having structurally frustrated Lewis pairs therein.

First claim

What is claimed is:

1. A hydrogenation process, comprising:
catalytically hydrogenating a compound having at least one functional group selected from the group consisting of carbonyls, nitriles, alkenes, alkynes, and combinations thereof, with a catalyst comprising a solid material comprising a sheet of catalytically active material having frustrated Lewis acid-base pairs along a surface of the sheet.

2. The process of claim 1 , wherein the compound comprises at least one carbonyl group.

3. The process of claim 2 , wherein the compound is carbon dioxide.

4. The process of claim 3 , wherein the hydrogenation of carbon dioxide produces formic acid.

5. The process of claim 1 , wherein the solid material having frustrated Lewis pairs comprises a solid surface having at least one Lewis acid site and at least one Lewis base site, and at least one defect frustrating at least one pair of Lewis acid and Lewis base sites, wherein the at least one frustrated pair of Lewis acid and Lewis base sites is catalytically active.

6. The process of claim 1 , wherein the solid material having frustrated Lewis pairs comprises a solid surface having Lewis acid moieties and Lewis base moieties spaced a distance apart from one another such that catalytic activity is present there-between and the formation of an acid-base adduct therefrom is prevented.

7. The process of claim 6 , wherein the Lewis acid moieties are selected from the group consisting of Group 13 elements in a trigonal planar configuration, halides of Group 15 elements, electron poor π-systems, and combinations thereof.

8. The process of claim 6 , wherein the Lewis base moieties are selected from the group consisting of simple anions, lone-pair-containing species, complex anions, electron rich π-systems, and combinations thereof.

9. The process of claim 6 , wherein the Lewis acid moieties are selected from the group consisting of Group 13 elements in a trigonal planar configuration, halides of Group 15 elements, electron poor π-systems, and combinations thereof, and the Lewis base moieties are selected from the group consisting of simple anions, lone-pair-containing species, complex anions, electron rich it-systems, and combinations thereof.

10. The process of claim 6 , wherein the Lewis acid moiety is a Group 13 element in a trigonal planar configuration and the Lewis base moiety is a lone-pair containing species.

11. The process of claim 6 , wherein the hydrogenation catalyst at least partially comprises hexagonal boron nitride.

12. The process of claim 1 , wherein the catalyst comprises hexagonal boron nitride having a catalytically active defect on a surface thereof.

13. The process of claim 12 , wherein the catalytically active defect is selected from the group consisting of Stone-Wales defects, B/N defects, boron substituted for nitrogen, nitrogen substituted for boron, carbon substituted for nitrogen, carbon substituted for boron, boron vacancy, nitrogen vacancy, and combinations thereof.

14. The process of claim 12 , wherein the catalytically active defect is boron substituted for nitrogen.

15. The process of claim 1 , wherein the compound has at least one functional group selected from the group consisting of carbonyls, nitriles, alkenes, and combinations thereof.

16. A hydrogenation process, comprising:
catalytically hydrogenating carbon dioxide with a catalyst comprising a solid material comprising a sheet of catalytically active material having frustrated Lewis pairs along a surface of the sheet, wherein the hydrogenation of the carbon dioxide coats at least one hydrocarbon onto the catalyst.

17. The process of claim 16 , wherein the at least one hydrocarbon is collected by heating the catalyst to a temperature greater than 100° C.

18. The process of claim 17 , wherein the catalyst is heated to a temperature greater than 400° C.

19. The process of claim 17 , wherein the catalyst is heated to a temperature greater than 800° C.

Assignees

• Univ Central Florida Res Found Inc

Inventors

• Blair Richard G

Classifications

• C07C51/00 Primary

  Preparation of carboxylic acids or their salts, halides or anhydrides (of acids by hydrolysis of oils, fats or waxes C11C) · CPC title

• B01J27/24

  Nitrogen compounds · CPC title

• C10G3/00

  Production of liquid hydrocarbon mixtures from oxygen-containing organic materials, e.g. fatty oils, fatty acids (production from non-melting solid oxygen-containing carbonaceous materials C10G1/00) · CPC title

• Y02P30/20

  using bio-feedstock · CPC title

• B01J37/0036

  Grinding · CPC title