PROCESS FOR MANUFACTURING A NITROGEN-CONTAINING POROUS CARBONACEOUS MATERIAL

• US 20130244862A1
• Filed: 11/24/2011
• Published: 09/19/2013
• Est. Priority Date: 11/26/2010
• Status: Abandoned Application

• Current Assignee: BASF SE, Max-Planck-Gesellschaft Zur Foerderung Der Wissenschaften e.V. (Max-Planck-Gesellschaft zur Frderung der Wissenschaften e)
• Original Assignee: BASF SE, Max-Planck-Gesellschaft Zur Foerderung Der Wissenschaften e.V. (Max-Planck-Gesellschaft zur Frderung der Wissenschaften e)
• Inventors: Ivanovici, Sorin, Muellen, Klaus, Schwab, Matthias, Yanyu, Liang
• Application Number:
  US13/988,895
• Publication Number:
  US 20130244862A1
• Time in Patent Office: Days
• US Class Current: 502/101
• CPC Class Codes: B01J 21/18 Carbon
• CPC Class Codes: B01J 35/617 500-1000 m2/g
• CPC Class Codes: B01J 35/618 more than 1000 m2/g
• CPC Class Codes: B01J 35/635 0.5-1.0 ml/g
• CPC Class Codes: B01J 35/638 more than 1.0 ml/g
• CPC Class Codes: B01J 35/647 2-50 nm
• CPC Class Codes: B01J 37/084 Decomposition of carbon-containing compounds into carbon
• CPC Class Codes: C01B 32/00 Carbon; Compounds thereof C01B21/00, C01B23/00 take precedence; percarbonates C01B15/10; carbon black C09C1/48
• CPC Class Codes: C01P 2006/12 Surface area
• CPC Class Codes: C01P 2006/14 Pore volume
• CPC Class Codes: C04B 2235/3895 Non-oxides with a defined oxygen content, e.g. SiOC, TiON
• CPC Class Codes: C04B 2235/72 Products characterised by the absence or the low content of specific components, e.g. alkali metal free alumina ceramics
• CPC Class Codes: C04B 35/532 containing a carbonisable binder
• CPC Class Codes: H01G 11/32 Carbon-based
• CPC Class Codes: H01G 11/84 Processes for the manufacture of hybrid or EDL capacitors, or components thereof
• CPC Class Codes: H01M 4/9008 Organic or organo-metallic compounds
• CPC Class Codes: Y02E 60/10 Energy storage using batteries
• CPC Class Codes: Y02E 60/13 Energy storage using capacitors
• CPC Class Codes: Y02E 60/50 Fuel cells

Abstract

Disclosed is a process for manufacturing a nitrogen-containing porous carbonaceous material with an optional inorganic salt content of up to 50 ppm by weight. The process comprises the following steps: (A) conversion of (a) at least one heterocyclic hydrocarbon with at least two NH2-groups per molecular with (b) at least one aromatic compound with at least two aldehyde groups per molecular, (B) heating in the absence of oxygen to temperature in the range of from 700 to 1200° C.

Claims

1. A process for manufacturing a porous carbonaceous material comprising nitrogen, with an optional inorganic salt content of up to 50 ppm by weight, the process comprising:

reacting

a heterocyclic hydrocarbon comprising at least two NH₂-groups per molecule with

an aromatic compound comprising at least two aldehyde groups per molecule, and

heating in an absence of oxygen to a temperature of from 700 to 1200°

C.,

wherein the aromatic compound comprises a backbone selected from the group consisting of a carbocyclic aromatic ring and a heterocyclic aromatic ring, and

the aldehyde groups are directly linked to the backbone.

2. The process according to claim 1, wherein the heterocyclic hydrocarbon is selected from heteroaromatic hydrocarbons with at least two NH₂-groups per molecule.

3. The process according to claim 1, wherein the aromatic compound is selected from the group consisting of heteroaromatic dialdehyde, heteroaromatic trialdehyde, carbocyclic aromatic dialdehyde, and carbocyclic aromatic trialdehyde, in which an aromatic backbone is selected from the group consisting of phenylene, naphthylene, biphenylene, fluorenylene, anthracenylene, pyrenylene, perylenylene, indenylenee, 1,1′

;

4′

,1″

-terphenylenylene, 1,1′

-spirobi[inden]ylene, and 9,9′

-spirobi[fluoren]ylen.

4. The process according to claim 1, wherein the aromatic compound is a heteroaromatic dialdehyde selected from molecules of formula (I) and (II)

5. The process according to claim 1, wherein the reacting is performed in DMSO as solvent.

6. The process according to claim 1, wherein the reacting does not comprise a catalyst comprising a metal ion.

7. The process according to 6claim 1, wherein the heterocyclic hydrocarbon is selected from compounds of formula (III),

8. A carbonaceous material having a nitrogen content of from 1 to 8% by weight and an optional inorganic salt content up to 50 ppm, a BET surface of from 500 to 700 m²/g and a capacitance of from 5 to 100 μ

F/cm².

9. The carbonaceous material according to claim 8, comprising fused aromatic and N-containing heteroaromatic rings.

10. The carbonaceous material according to claim 8, wherein the carbonaceous material has a total pore volume of from 0.1 to 3.0 cm³/g, determined by nitrogen adsorption method essentially according to DIN 66135.

11. The carbonaceous material according to claim 8, wherein the carbonaceous material has a total sulphur content of from 0.1 to 1.0% by weight.

12. The carbonaceous material according to claim 8, wherein the carbonaceous material is obtained by a process comprising:

reacting a heterocyclic hydrocarbon comprising at least two NH₂-groups per molecule with an aromatic compound comprising at least two aldehyde groups per molecule, and

heating in an absence of oxygen to a temperature of from 700 to 1200°

C.,

wherein the aromatic compound comprises a backbone selected from the group consisting of a carbocyclic aromatic ring and a heterocyclic aromatic ring, and

the aldehyde groups are directly linked to the backbone.

13. The carbonaceous material according to claim 8, wherein the material is suitable for capacitors.

14. The carbonaceous material according to claim 8, wherein the material is suitable as a catalyst or as a support for catalysts.

15. A catalyst comprising a carbonaceous material according to claim 8.

16. An electrode comprising carbonaceous material according to claim 8 and at least one a binder.

17. The electrode according to claim 16, further comprising an additive.

18. A process for manufacturing electrodes according to claim 16, the process comprising:

mixing a carbonaceous material with a binder and optionally an additive in the presence of water to obtain a mixture;

applying the mixture to a metal filmy and

drying

wherein the carbonaceous material has a nitrogen content of from 1 to 8% by weight, an optional inorganic salt content up to 50 ppm, a BET surface of from 500 to 700 m²/g, and a capacitance of from 5 to 100 μ

F/cm².