US4634546A
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US
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Process for the intercalation of graphitic carbon employing fully halogenated hydrocarbons
Assignee: Celanese Corp
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Filing: 1985-07-19
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Granted: 1987-01-06
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Expires: 2005-07-19
Abstract
Abstract An improved procedure is provided for increasing the electrical conductivity of graphite via intercalation. It has been found that fully halogenated hydrocarbons (as described) have the ability to substantially aid the intercalation of graphite by previously known intercalant mixtures of (a) fluorosulfonic acid, chlorosulfonic acid, or mixtures thereof, and (b) a boron trihalide, a tetrahalide of a Group IV element, a pentahalide of a Group V element, or mixtures thereof. The presence of a fully halogenated hydrocarbon, such as carbon tetrachloride, during the graphite intercalation reaction has been found to expedite the rate at which intercalation takes place and possibly enables the achievement of a greater electrical conductivity than would have otherwise been obtained. In a preferred embodiment the graphite carbon is present within a carbonaceous fibrous material at the time of its intercalation and the resulting product is substantially electrically oriented along the axis of the fiber.
Inventors
- 👤 Ilmar L. Kalnin
- 👤 Harris A. Goldberg
- 👤 George J. Breckenridge, Jr.
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-09 06:13
CPC Classifications
H; H01; H01B; H01B1/00; H01B1/04; C; C01; C01B; C01B32/00; C01B32/20; C01B32/21; C01B32/22
Claims Analysis
Total Claims: 30
Claim 1
Independent Claim
170 words
In a process for forming an intercalated electrically conducting composition comprising reacting graphite in a reaction zone under anhydrous conditions with: (a) sulfur-containing reactant selected from the group consisting of fluorosulfonic acid, chlorosulfonic acid, and mixtures thereof, and (b) a halide reactant selected from the group consisting of boron trihalide, a tetrahalide of a Group IV element, a pentahalide of a Group V element, and mixtures thereof; the improvement of additionally providing in said reaction zone while at a temperature of a approximately 0° to 50° C. during at least a portion of said reaction a fully halogenated hydrocarbon having 1 to 4 carbon atoms which is capable of aiding the increase in the electrical conductivity of the graphite, wherein contact between said halide reactant (b) and said fully halogenated hydrocarbon for more than about 30 minutes prior to contact with said graphite is avoided, and wherein the molar ratios of reactant (a), reactant (b), and the fully halogenated hydrocarbon provided in the reaction zone are approximately 1:0.1:100 to 100:20:100.
Claim 2
Dependent Claim
170 words
In a process for forming an intercalated electrically conducting composition comprising reacting graphite in a reaction zone under anhydrous conditions with: (a) sulfur-containing reactant selected from the group consisting of fluorosulfonic acid, chlorosulfonic acid, and mixtures thereof, and (b) a halide reactant selected from the group consisting of boron trihalide, a tetrahalide of a Group IV element, a pentahalide of a Group V element, and mixtures thereof; the improvement of additionally providing in said reaction zone while at a temperature of a approximately 0° to 50° C. during at least a portion of said reaction a fully halogenated hydrocarbon having 1 to 4 carbon atoms which is capable of aiding the increase in the electrical conductivity of the graphite, wherein contact between said halide reactant (b) and said fully halogenated hydrocarbon for more than about 30 minutes prior to contact with said graphite is avoided, and wherein the molar ratios of reactant (a), reactant (b), and the fully halogenated hydrocarbon provided in the reaction zone are approximately 1:0.1:100 to 100:20:100.
Claim 3
Dependent Claim
36 words
A process for forming an intercalated electrically conducting composition according to claim 1 wherein said graphite is in the form of a fiber and the resulting intercalated electrically conducting composition is electrically oriented along its axis.
Claim 4
Dependent Claim
22 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein said sulfur-containing reactant (a) is fluorosulfonic acid.
Claim 5
Dependent Claim
22 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein said halide reactant (b) is a fluoride.
Claim 6
Dependent Claim
43 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein said halide reactant (b) is a Group IV element tetrahalide selected from the group consisting of SiF 4 , HfF 4 , TiF 4 and ZrF 4 .
Claim 7
Dependent Claim
45 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein said halide reactant (b) is a Group V element pentahalide selected from the group consisting of PF 5 , NbF 5 , TaF 5 AsF 5 and SbF 5 .
Claim 8
Dependent Claim
22 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein said halide reactant (b) is antimony pentafluoride.
Claim 9
Dependent Claim
31 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein said sulfur-containing reactant (a) is fluorosulfonic acid and said halide reactant (b) is SbF 5 .
Claim 10
Dependent Claim
51 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein said fully halogenated hydrocarbon possesses the formula C n X 2n+2 where n is a whole number from 1 to 4 and X is selected from the group consisting of F, Cl, Br, and mixtures thereof.
Claim 11
Dependent Claim
43 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein said fully halogenated hydrocarbon is selected from the group consisting of carbon tetrachloride, fluorotrichloromethane, dichlorodifluoromethane, bromotrichloromethane, dibromochlorofluoromethane, 1,1,2-trichlorotrifluoroethane, tetrachlorodifluoroethane, trichloropentafluoropropane, tetrachlorotetrafluoropropane, octachloro-1,4-difluorobutane, hexachloro-1,3-butadiene, and mixtures of the foregoing.
Claim 12
Dependent Claim
22 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein said fully halogenated hydrocarbon is carbon tetrachloride.
Claim 13
Dependent Claim
39 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein contact between said halide reactant and said fully halogenated hydrocarbon for more than about 15 minutes prefer to contact with said graphite is avoided.
Claim 14
Dependent Claim
38 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein the molar ratios of reactant (a), reactant (b), and the fully halogenated hydrocarbon provided in the reaction zone are approximately 10:1:100 to 50:10:100.
Claim 15
Dependent Claim
38 words
An improved process for forming an intercalated electrically conducting composition according to claim 1 wherein the contents of said reaction zone are provided at a temperature of approximately 15° to 35° C. during the course of said reaction.
Claim 16
Dependent Claim
175 words
An improved process for forming an intercalated electrically conducting fiber which is electrically oriented along its axis comprising reacting in an reaction zone under anhydrous conditions while at a temperature of approximately 0° to 50° C. a carbonaceous fibrous material comprising graphitic carbon with the following reactants: (a) a sulfur-containing reactant selected from the group consisting of fluorosulfonic acid, chlorosulfonic acid, and mixtures thereof, (b) a halide reactant selected from the group consisting of boron trihalide, a tetrahalide of a Group IV element, a pentahalide of a Group V element, and mixtures thereof, and (c) a fully halogenated hydrocarbon having 1 to 4 carbon atoms, wherein the fully halogenated hydrocarbon is capable of substantially aiding the increase in the electrical conductivity of the carbonaceous fibrous material comprising graphitic carbon, contact between said halide reactant (b) and said fully halogenated hydrocarbon (c) for more than about 30 minutes prior to contact with said graphite is avoided, and the molar ratios of reactants (a), (b) and (c) provided in the reaction zone are approximately 1:0.1:100 to 100:20:100.
Claim 17
Dependent Claim
175 words
An improved process for forming an intercalated electrically conducting fiber which is electrically oriented along its axis comprising reacting in an reaction zone under anhydrous conditions while at a temperature of approximately 0° to 50° C. a carbonaceous fibrous material comprising graphitic carbon with the following reactants: (a) a sulfur-containing reactant selected from the group consisting of fluorosulfonic acid, chlorosulfonic acid, and mixtures thereof, (b) a halide reactant selected from the group consisting of boron trihalide, a tetrahalide of a Group IV element, a pentahalide of a Group V element, and mixtures thereof, and (c) a fully halogenated hydrocarbon having 1 to 4 carbon atoms, wherein the fully halogenated hydrocarbon is capable of substantially aiding the increase in the electrical conductivity of the carbonaceous fibrous material comprising graphitic carbon, contact between said halide reactant (b) and said fully halogenated hydrocarbon (c) for more than about 30 minutes prior to contact with said graphite is avoided, and the molar ratios of reactants (a), (b) and (c) provided in the reaction zone are approximately 1:0.1:100 to 100:20:100.
Claim 18
Dependent Claim
27 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material comprising graphitic carbon according to claim 15 wherein said sulfur-containing reactant (a) is fluorosulfonic acid.
Claim 19
Dependent Claim
27 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 comprising graphitic carbon wherein said halide reactant (b) is a fluoride.
Claim 20
Dependent Claim
44 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 wherein said reactant (b) is a Group IV element tetrahalide selected from the group consisting of SiF 4 , HfF 4 , TiF 4 and ZrF 4 .
Claim 21
Dependent Claim
47 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 wherein said reactant (b) is a Group V element pentahalide selected from the group consisting of PF 5 , NbF 5 , TaF 5 , AsF 5 and SbF 5 .
Claim 22
Dependent Claim
23 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 wherein said reactant (b) is antimony pentafluoride.
Claim 23
Dependent Claim
33 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 wherein said sulfur-containing reactant (a) is fluorosulfonic acid and the halide reactant (b) is SbF 5 .
Claim 24
Dependent Claim
53 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 wherein said fully halogenated hydrocarbon possesses the formula C n X 2n+2 where n is a whole number from 1 to 4 and X is selected from the group consisting of F, Cl, Br, and mixtures thereof.
Claim 25
Dependent Claim
45 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 wherein said fully halogenated hydrocarbon is selected from the group consisting of carbon tetrachloride, fluorotrichloromethane, dichlorodifluoromethane, bromotrichloromethane, dibromochlorofluoromethane, 1,1,2-trichlorotrifluoroethane, tetrachlorodifluoroethane, trichloropentafluoropropane, tetrachlorotetrafluoropropane, octachloro-1,4-difluorobutane, hexachloro-1,3-butadiene, and mixtures of the foregoing.
Claim 26
Dependent Claim
24 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 wherein said fully halogenated hydrocarbon is carbon tetrachloride.
Claim 27
Dependent Claim
41 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 wherein contact between said halide reactant and said fully halogenated hydrocarbon for more than about 15 minutes prior to contact with said graphite is avoided.
Claim 28
Dependent Claim
34 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 wherein the molar ratios of reactants (a), (b) and (c) provided in the reaction zone are approximately 20:1:100.
Claim 29
Dependent Claim
36 words
An improved process for forming an intercalated electrically conducting carbonaceous fibrous material according to claim 15 where the molar ratios of reactants (a), (b) and (c) provided in the reaction zone are approximately 10:1:100 to 50:10:100.
Claim 30
Dependent Claim
38 words
An improved process for forming an intercalated electrically conducting composition according to claim 15 wherein the contents of said reaction zone are provided at a temperature of approximately 15° to 35° C. during the course of said reaction.
References Cited (Backward Citations)
USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
|---|---|---|---|---|---|
| 3.5 Years (Year 4) | 1990-01-05 | 1990-07-07 | 1991-01-06 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1994-01-05 | 1994-07-07 | 1995-01-06 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 1998-01-05 | 1998-07-07 | 1999-01-06 | $7700.00 | Window Closed / Lapsed |