JPS5860607A - Interlaminar compound in graphite of aluminum fluoride and fluorine and its preparation - Google Patents

Abstract

PURPOSE:To provide a three-component graphite interlaminar compound composed of graphite, AlF3 and F, stable to moisture, and having excellent electrical conductivity. CONSTITUTION:Natural graphite or artificial graphite obtained by the thermal treatment of petroleum coke, etc. is made to contact with AlF3 in fluorine atmosphere at 0-400 deg.C at least until the weight of the graphite beings to increase. After the completion of the reaction, the temperature of the reaction system is lowered to the room temperature, and the unreacted AlF3 is separated from the system to obtain the objective three-component graphite interlaminar compound of formula CxF(AlF3)y. There are 4 stages in the graphite interlaminar compound, and the periodic distance Ic of CxF(Al)y is 9.4-9.5Angstrom at the 1st stage, 12.8-12.9 Angstrom at the 2nd stage, 16.1-16.2Angstrom at the 3rd stage, and 19.5-19.6Angstrom at the 4th stage. The three-component graphite interlaminar compound has high heat resistance as well as the above-mentioned characteristics.

Description

DETAILED DESCRIPTION OF THE INVENTION In particular, the present invention relates to a moisture-stable graphite intercalation compound obtained by reacting aluminum fluoride, fluorine, and graphite under specific conditions. The present invention also relates to a method for producing such a novel graphite intercalation compound.

In recent years, fluoride graphite intercalation compounds have been attracting attention because of their excellent electrical conductivity. However, most of them are hygroscopic and unstable, making it extremely difficult to use them practically. Until now, fluoride, which has been known as an intercalating substance that creates graphite intercalation compounds, has a low melting point and boiling point, and is gaseous or liquid at room temperature.Fluoride, which is an intercalating substance, generally has a high vapor pressure at a relatively low temperature. The conventional wisdom was that this was necessary. Therefore, no attempt has been made to produce a graphite intercalation compound of fluoride having a high melting point or boiling point. In fact, a binary graphite intercalation compound of aluminum fluoride and graphite, which exhibits no vapor pressure even at high temperatures, is not produced.

However, as a result of research on iron content, the present inventors found that by reacting under specific conditions, a ternary graphite interlayer mixture of aluminum fluoride, fluorine, and graphite has a ratio of 100 to graphite. The graphite intercalation compound obtained is not only stable against moisture but also has high heat resistance, and has an excellent electrical conductivity that is an order of magnitude higher than that of the raw material graphite. The present invention was achieved based on the discovery that this is the case.

Therefore, it is an object of the present invention to provide a novel graphite intercalation compound of aluminum fluoride and turronite.

Another object of the present invention is to provide a method for producing this novel graphite intercalation compound.

These and other features and benefits of the present invention will become apparent from the following detailed description and accompanying drawings.

According to one (') aspect of the invention, the formula CxF(AlF2
) A graphite intercalation compound with aluminum fluoride and fluorine, represented by y, is provided.

The graphite intercalation compound represented by the above formula is a typical example of the graphite intercalation compound of aluminum fluoride and fluorine according to the present invention. ! : A mixture of fluoride and carbide was heated in a fluorine atmosphere for about 20 minutes.
Reaction at a temperature of ~400°C is an essential requirement for obtaining the graphite intercalation compound of the present invention.

The graphite intercalation compound of the present invention represented by the formula CxF(AlF2)y includes those having two or more stehs: a first steh, a second steh, a third steh, or more. For the first steno, x = 2 ~ l7, y = 0.002 ~ 0
．． It is 45. The values of X and y are influenced by the holding time and fluorine pressure after fluorine is introduced into the mixture of aluminum fluoride and graphite raw materials, which will be described later. For the second steno, x=17-50, y=0.002-0.
It is 45. For the 3rd steno or higher, X〉30
, y=lQ ~10. The number of stays 2 is determined from the periodic distance (Ie) obtained from X-ray diffraction.

Next, the manufacturing method will be specifically explained.

A mixture of graphite raw material H and aluminum fluoride was put into a nickel reactor and heated for 5 to 30 minutes.

Introduce elementary gas. In that case, the temperature is about 20-100℃
The range shall be . After introducing the fluorine gas and maintaining the temperature for 0 to 1 hour, the temperature is raised at a rate of 111j of 2° C./min to 10° C./min, and the reaction is carried out at a temperature of 300 to 400° C. for about 20 hours to 31 hours. Generally, aluminum fluoride is used in an excessive amount, so after the reaction is completed, it is separated using a sieve to obtain the target graphite intercalation compound of aluminum fluoride and fluorine. The graphite intercalation compound obtained in this way is of the first steno type, has a blue-black color, and its X-ray diffraction pattern does not change even if it is left in the air for several days or soaked in water overnight. It was fairly stable. It was found that the periodic distance was 94 to 9.5X from the (002) diffraction line.

Instead of the above method (temperature raising method), if a mixture of graphite raw material and aluminum fluoride is placed in a nickel cracking reactor, fluorine gas is introduced at a temperature of about 20 to 100 degrees Celsius, and it is left as it is for more than 20 hours. The intercalation compound of the first stage is not obtained, and what is obtained is a mixture of different stages of the second stage or higher, or sometimes an intercalation compound of the second stage is obtained. The periodic distance of the second stage is 12.8-12.9, and that of the third stage is 1
61-162, that of the 4th steno is 19.5-196
It is. The intercalation compound having the number of stages equal to or higher than the second stage is black and is also stable.

As the graphite raw material used in the present invention, in addition to natural graphite, artificial graphite obtained by heat treating petroleum coke or the like can also be used. The particle size is not critical and flakes or powders can be used, i.e. about 20
~50 meters or even more than 400 meters can be used. In addition, in special cases, when block-shaped objects are buried, methane,
Hydrocarbons such as fluorine, benzene, and acetylene can be decomposed and deposited on a substrate at about 2,100° C., followed by heat treatment. In that case,
Different degrees of graphitization are obtained depending on the heat treatment temperature, and those treated at about 2.400°C are pyrolytic carbon (hereinafter referred to as PC) -1 from about 2,600°C to about 3,000°C.
The material treated at 0℃ is pyrolytic graphite (
(hereinafter referred to as PG).

In the case of PC, a fourth steno intercalation compound can be obtained by setting the holding time after fluorine introduction to about 24 hours in the above-mentioned Gar temperature method. The product is designated PCF(AlF2)y, where y is as previously described.

In the case of PC, the first steno product can be obtained with a retention time of about 1 hour. In addition, in the case of PG, a second steno type can also be obtained. The product is designated PGF(AlF2)y, where y is as previously described.

In carrying out the production method of the present invention, the fluorine pressure is not particularly critical, but approximately 0.5 to 10 atm is used; however, when the fluorine pressure is 5 atm or more, CxF(A
lF2) Indicates the direction in which the X of y becomes ・j・smaller. The weight/l ratio of the graphite raw material and the aluminum fluoride used is 1:1 to 1:10 when the first steno is the target material,
The amount of aluminum fluoride may be small. If you are aiming for the second steno, 1:o, 5th place may be sufficient.

Although the above explanation was made using the punch method C', it is natural that a continuous production method using the flow method is possible.

Next, typical analytical values for CF(AlF2)y are shown in Table 1. , 15 X-ray diffraction diagram of fluorinated graphite (02F). This is shown in comparison with that of . Also, C,
, F(/d3). ,. .

From Figure 2 showing the DTA curve of CxF(AlF2),
It can be seen that decomposition begins at around 150°C. The third factor shows the ESCA spectrum, and the first steno is graphite fluoride (02F). It is similar to that of the C-F covalent bond near the q' and 'ivc surfaces.
A peak is observed at 289 cV.

Next, Examples of the present invention will be described, but it is clear from the various data described above that the scope of the present invention is not limited to the Examples.

Example Flake-like natural graphite from Madakascar (297-840
/1m ) 0.3 g- and powdered AtF60.6!
i' was mixed, placed in a Ni reaction tube, and evacuated. Add to this at room temperature.

Introduce elementary gas to 1 atm, leave for 30 minutes and then heat to 350°C
The temperature was raised at a rate of 1° C./min until the temperature reached 1° C., and the reaction was allowed to proceed for 30 hours. After the reaction is completed, the excess AtF% is separated using a 297 μm sheep and the blue-black 06F (AlF2) is obtained. ,,5
I got it.

[Brief explanation of drawings]

Figure 1 shows C6F (AlF2). , 15 and (02F)n, and Figure 2 is 011F (AlF2). ,
. Figure 3 shows the intercalation compound of the present invention and (C, F). This is the ESCA spectrum of Patent applicant: Central Glass Co., Ltd. Engraving of drawings (no change in content) Diffraction 2e (') Cheating ('C) 295 290 285 280 695 690
685R4'':i;'fuz\'-(eV) Procedural amendment (炕荀) 170th month of the Showa era. r+
1"3%'T7Q (1) Et name (name) (zlO)
1985 FH'l JHI: 3 Supplement 11 Relationship with the 11 cases Patent applicant (-t'゛- 5253 Oki-Ube, Ube City, Yamaguchi Prefecture) (Name) (220) Central Glass Co., Ltd. 1
6. Number of inventions to be increased by supplementary IF 17. Subject of amendment Full text of the amendment 1. Name of the invention A ternary graphite intercalation compound of graphite, aluminum fluoride, and fluorine, a method for producing the same, and an electrically conductive material made from the same 2 Claims<1) A ternary graphite intercalation compound of graphite, aluminum fluoride, and fluorine represented by the formula CxF(AlF2)y. (2) X is about 3 to 100 and y is about 0.0001 to 020
The ternary graphite intercalation compound according to claim (1), which is characterized in that: (3) The ternary graphite intercalation compound comprises a first steno compound, a second stage compound, a third stage compound, and a steno compound, a second stage compound, a third stage compound, and a third stage compound.
at least two selected from the group consisting of one-stage compounds;
3. The ternary graphite intercalation compound according to claim 1, which is a mixed-stage compound comprising seeds. (4) A time period A in which the raw material graphite is exposed to a fluorine atmosphere at a temperature of 0 to 400°C to at least cause the graphite to increase in weight.
The formula CxF(At
F.) A method for producing a ternary graphite intercalation compound of graphite, aluminum fluoride, and fluorine represented by y. (5) Raw materials graphite and aluminum fluoride Nff1
The method according to item (4), characterized in that the ratio is 1:(1.4 to 1:10).(6) The method is characterized in that the temperature is 15 to 370°C. The method according to claim (4). (7) The fluorine pressure of the fluorine atmosphere is 05 to 10 atm.
The method according to claim (4), characterized in that: (8) An electrically conductive material made of a ternary graphite intercalation compound of graphite, aluminum fluoride, and fluorine that is blued by the formula CxF(AtF3)y. 3. Detailed Description of the Invention In detail, the present invention relates to a ternary graphite intercalation compound of graphite, aluminum fluoride, and fluorine, which is not only stable against moisture but also has excellent electrical conductivity. The present invention also relates to a method for producing a ternary graphite intercalation compound of graphite, aluminum fluoride, and fluorine. The present invention also relates to a conductive material comprising a ternary graphite intercalation compound of graphite, aluminum fluoride, and fluorine. In recent years, fluoride graphite intercalation compounds have been attracting attention because of their excellent electrical conductivity. However, most of the conventionally known graphite intercalation compounds are unstable to moisture and therefore decompose immediately when left in the air. Therefore, it is impossible to put it into practical use. Fluoride, which has so far been used as an intercalant to create graphite intercalation compounds, has a low melting point and boiling point, and is gaseous or liquid at room temperature. Therefore, it has been generally accepted that fluoride as an interstitial substance needs to have a relatively low temperature and high vapor pressure. Therefore, no attempt has been made to produce a graphite intercalation compound of fluoride having a high melting point or boiling point. Most importantly, a binary graphite intercalation compound of aluminum fluoride and graphite, which exhibits no vapor pressure even at high temperatures, is not generated. The present inventors have conducted extensive research to develop a practically usable fluoride graphite intercalation compound that not only has excellent conductivity but is also extremely stable against moisture, and as a result, has developed a graphite intercalation compound of the formula CxF (AtFρ, A ternary graphite intercalation compound of graphite, aluminum fluoride, and fluorine (hereinafter often simply referred to as ``ternary graphite intercalation compound'') expressed by The obtained ternary graphite intercalation compound is not only stable against moisture but also has high heat resistance and excellent electrical conductivity. The electrical conductivity is one order of magnitude higher than that of raw material graphite.The present invention was made based on this new knowledge.Therefore, the object of the present invention is to not only be stable against moisture, but also to be stable against moisture. It is an object of the present invention to provide a novel ternary graphite intercalation compound that has high heat resistance and excellent conductivity. Another object of the present invention is to provide a method for producing this novel ternary graphite intercalation compound. Another object of the present invention is to provide a novel electrically conductive material comprising the novel ternary graphite intercalation compound as described above. The features and benefits of the invention will become apparent from the following detailed description and accompanying drawings. A ternary graphite intercalation compound is provided. Generally, a ternary graphite having the formula CxF(AtF3), The intercalation compound is obtained by contacting raw graphite with AtF in a fluorine atmosphere at a temperature of 0 to 400°C for at least a period of time to cause a weight increase in the graphite.Hereinafter, the present invention will be explained in detail. The ternary graphite intercalation compound of the present invention represented by the formula CxF(AtF,) includes a first steno stage, a second stage,
There is a third steno, a fourth steno, or more stages. The stake number of the ternary graphite intercalation compound is determined by measuring the periodic distance (IC) obtained from X-ray diffraction. The number of stakes of the obtained ternary graphite intercalation compound is influenced not only by the reaction temperature and time but also by the crystallinity and thickness (in the C-axis direction) of the raw graphite. For the first stethoscope, X=approximately 30-20 and y=approximately 0.03-020. For the second stethoscope, x=approximately 11 to 50, y=approximately (1,01 to
It is 0.15. For stage 3 and above, X - about 3
0 to 60, and y=10-' to 10-2. In the ternary graphite intercalation compound generally represented by the formula CxF(AtF3)y, X is about 3-100 and y is about 0.0001-020. For each of the first stage, second stage, second stage, and fourth stage or higher stage compounds, X and y
The value varies within the above-mentioned range not only by the reaction temperature and time but also by the crystallinity of the raw material graphite and the thickness in the C-axis direction. As the graphite raw material used in the present invention, in addition to natural graphite, artificial graphite obtained by heat treating petroleum coke or the like can also be used. The particle size is not critical and is flake-like or powder-like, about 20 to 50 mm, shumata (d50 to
A material having 400 meshes or more than 400 meshes (Tyler) can be used. Alternatively, if block-shaped graphite is desired, hydrocarbons such as methane, propane, benzene, chickpeas, or acetylene are brought into contact with a substrate (generally made of artificial graphite) heated to about 2,100 C to carbonize the graphite. A material obtained by thermally decomposing hydrogen, depositing the obtained graphite material on a base material, and then heat-treating the deposited graphite material can be used. In that case, block-shaped graphite having different degrees of graphitization can be obtained depending on the heat treatment temperature. Approximately 2.
Heat treatment at 490° C. gives a pyrotic carbon layer. When heat-treated at a temperature of about 2,600°C to 3,000°C, pyrotic graphite having higher crystallinity than pyrotic carbon can be obtained. The raw material graphite is heated in a fluorine atmosphere at a temperature of 0 to 4001? . When causing at least a weight increase in the graphite at l:i
For the production of a ternary graphite intercalation compound of the formula CxF(AtF3)y by contacting with JAZFs, the preferred reaction conditions are as follows. Fluorine pressure is not particularly critical, but is usually 0.5-1
Around 0 atm is used. The reaction temperature is 0 to 400°C, preferably 15 to 370°C. As mentioned above, the formula CxF(A7F5), with the desired y and y values,
The reaction time required to obtain the compound represented by is dependent on the crystallinity of the raw graphite, the thickness in the C@ force direction, and the reaction temperature. However, reaction times are generally from 1 hour to 10 months, more generally from 1 day to 8 days. The weight ratio of raw material graphite to AtF3 depends on the desired number of stakes of the ternary graphite intercalation compound, but is usually 1:0.4 to 1:10. What should be noted about the reaction conditions is that the temperature of the reaction system is 100
When the temperature is raised to higher than 100°C, an increase in weight of graphite is observed when the temperature drops below 100°C in the process of cooling the once-heated reaction system. It is often a compound with a high Steso number in the C-axis direction of raw graphite. To obtain the first steno compound, usually
It is preferable to use a graphite material with a thickness (in the C-axis direction) of up to 0, s mm. After the reaction is completed, if the temperature of the reaction system has been raised to a temperature higher than room temperature, the temperature of the reaction system is lowered to room temperature. Unreacted AtF5 is separated by a sieve or pinscent to obtain the desired ternary graphite intercalation compound represented by the formula CxF(AtF,)y. The periodic distance (IC) of CXF(AtF3)y is 94-9.5X for the first steno, 12.8-12.9X for the second steno, and 16 for the third steno. .1-16.2X1 and 19.5-19.6X for the fourth stage. In the case of a ternary graphite intercalation compound represented by the formula cxF(AtF5)y, the first steno compound exhibits a blue-black to black color, and the second, third, and third steno compounds exhibit a blue-black to black color. and the fourth steno compound exhibits black color. 3 according to the present invention represented by the formula CxF(AtF3)y
All component-based graphite intercalation compounds are extremely stable against moisture, so even if they are left in the air for several weeks or soaked in water overnight, no change is observed in their X-ray diffraction patterns. do not have. Table 1 shows the results of elemental analysis and X-ray diffraction of some examples of the ternary graphite intercalation compound of the present invention represented by the formula CxF(Alt5). Table 1 Figure 1 shows the X-ray diffraction diagram 6 of CF (A7.F).
3 0.15 (Cu-) to (C2F). 71% by weight and (CF
). It is shown in comparison with that of fluorinated graphite consisting of 29 heavy suspensions. When considering the X-ray diffraction pattern of the ternary graphite intercalation compound described in -F, broad diffraction lines are sometimes observed. The periodic distance (IC) for one of the compounds represented by CxF(A/:F”3)y shown in FIG. 1 is (0
02) Calculated from the diffraction line and is 94X. In FIG. 2, C11F (AtF5). ,. The DTA curve of No. 9 (measured in air at a heating rate jJi: 20° C./min) is shown. In FIG. 2, 011F (AtF3). ,. A broad exothermic peak of No. 9 is observed to first start around 230°C. ESCA is one of the most useful tools to obtain valuable information about the chemical bond between host graphite and interloping substances. FIG. 3 shows the first stetho compound [C6F(AtF3). , 15] and CXF
ESCA of the second steno compound of (AtF3)y 02F) n71 weight if % and (CF)n2
This is shown in comparison with that of fluorinated graphite, which is composed of 9-layered carbon atoms. On the other hand, the 18 peak of carbon is 28Q, 9eV
and 287. (Two are observed at l eV.28
9. The C1S peak observed at OeV is C-F
The C1S peak observed at 287, OeV is derived from the C-C bond adjacent to the C-F bond.
It originates from bonding. (CF) type fluorinated graphite has only C-C bonds, so its ESCA spectrum is 289. It has only one 013 peak at OeV. For the second steno compound, a strong peak is observed at 2840e■ with a broad shoulder over the range from 286eV to 291eV. The latter suggests the presence of fluorine atoms chemically adsorbed and covalently bonded to the carbon atoms of the host graphite. The FIS spectrum also has a relatively broad peak at 687.6 eV. C6F(A/-F5). , 15, the C+S peak is observed at the same position as fluorinated graphite, but this is because most of the chemical bonds between the host graphite and the interstitial fluorine are (C,F).
Similar to that of n, 1 to 7 indicate a covalent bond. In ESCA consideration, the kinetic energy of photoelectrons emitted from the inner shell of each atom is measured. Since the mean free path of photoelectrons in a solid is at most a few dozen layers, only a few graphite layers can be analyzed in graphite intercalation compounds. Therefore, the chemical bonds near the surface of the compound are ESC
In the A sequence ξ vector, 1 appears strongly. Comparing the intensities of the peaks of the analyzed chemical compositions, it can be seen that graphite fluoride (tii) is generated near the surface of the first stage compound. Regarding the formation of the component-based graphite intercalation compound, the following is considered: The gas line (AtF, )m・(F2) is first generated by the reaction between AtF3 and fluorine, which is expressed by the following formula: mAtF - , + n F 22 (AtF 3 )m
(F2) The above gas line then penetrates the graphite. As the temperature increases, the chemical equilibrium shifts to the left, and the gaseous complex decomposes at high temperature. Even if a component-based graphite layer-opening compound is left in the air for several weeks7 and then analyzed by X-ray diffraction, almost the same X-ray diffraction and ξ turns can be obtained as if it were not left in the air. The ternary graphite intercalation compound according to the invention is stable against moisture, unlike conventional fluoride-graphite intercalation compounds which decompose immediately when left in air. Regarding the conductivity in the a-axis direction (direction perpendicular to the graphite layer), it is generally known to those skilled in the art that there is no substantial difference in conductivity between the second stage compound and the third steno compound. and 'r of the second steno, third stage compound.
It is known that the 1% concentration is superior to that of other stage compounds [Pouy Billand,
Ny Erold and F. Folk Le, Nnseti;
Metals No. 3 (1981). Pages 279-288 (D, B111 and A,
H5rold and F, Vogel. 5YNT) (ETICMETALS, 3 (1981
) 279-288)]. The ternary graphite intercalation compound according to the invention is not only stable against moisture but also has high electrical conductivity. According to the present invention: Ternary graphite intercalation compound (1) It can be used as a conductive material by wrapping it in copper foil or incorporating it into epoxy etc. The ternary graphite intercalation compound according to the present invention is useful as a conductive material. In addition, it can also be used as a catalyst in various organic reactions. Examples of the present invention will be described next, but the scope of the present invention is not limited to the examples. Example Madagascar flakes Natural graphite (297-840
/lrn ) 0.3 F and powdered AtF30.69 are mixed, placed in a Ni reaction tube, and evacuated. Fluorine gas was introduced into the mixture at a temperature of 25°C to create a pressure of 1 atm, and after the mixture was left to stand for 30 minutes, the temperature was raised at a rate of 4°C/min in a 350°C trench, and the mixture was allowed to react for 30 hours. Next, the reaction tube was cooled in a 25°C trench. Fluorine gas was replaced with nitrogen. After the reaction is completed, the product and unreacted AAF3 are separated using a 2971tm tube.
Blue-black graphite intercalation compound 06F (AAF5). I got 1.5. By the way, the ESCA consideration described here is based on Dupono's 6
This was carried out using a Mg-Ka beam using a 50B electron spectrometer. For DTA, CX-At in air
20. was performed as a control. A7 was analyzed by single atom absorption method. ” From the two series of examples, it is clear that the present invention has the formula CxF(AAF5)y
It is clear that the present invention provides a novel graphite intercalation compound having excellent properties and a method for producing the same. However, the features and benefits of the present invention are apparent from the extensive experimental data cited in conjunction with the foregoing detailed description. 4 Brief description of the drawings Fig. 1 shows C6F (AAF, , ), which is an example of the ternary graphite intercalation compound according to the present invention. ,,5. This is shown in comparison with that of carbonized graphite. FIG. 2 shows another example of a ternary graphite intercalation compound according to the present invention, C4. F(A,/F5). ,. 9 D
TA [itl line is shown. Figure: ES of the first stage and second stage compounds of the present invention containing AtF as the metal fluoride, respectively.
This is shown in comparison with that of fluorinated graphite coated with CA. Patent applicant: Central Nitto F Co., Ltd.

Claims (8)

[Claims] (1) A graphite intercalation compound of aluminum fluoride and fluorine represented by the formula CXF(AtF3)y. (2) A graphite intercalation compound with aluminum fluoride and fluorine represented by the formula PCF(AtF,)y (where pc is pyrolytic carbon). (3) A graphite intercalation compound with aluminum fluoride and fluorine represented by the formula PGF(AtF5)y (in the formula, PC is pyrolytic graphite). (4) A method for producing a graphite intercalation compound of aluminum fluoride and fluorine, which comprises reacting a mixture of graphite raw material and aluminum fluoride in a fluorine atmosphere at a temperature of about 20 to 40°C. (5) The graphite raw material is flake or powder graphite,
The mixture is kept under a fluorine atmosphere at a temperature of about 20 to 100°C for about 5 to 60 minutes, and then heated at a rate of about 2 to IOV minutes, and reacted at a temperature of about 300 to 400°C. ,
5. Process according to claim 4, characterized in that the product is CxF(AtF3)y. (6) The graphite raw material is flake or powder graphite,
The mixture is left to react under a fluorine atmosphere at a temperature of about 20 to 100°C for at least about 20 hours, and the product is CXF (A
Claim 4 characterized in that tF3)y
The method described in section. (7) The graphite raw material is NO9 yrolytic carbon, and after holding the mixture in a fluorine atmosphere at a temperature of about 20 to 100 °C for at least about 24 hours, the graphite raw material is
The temperature was raised at a temperature increase rate of 0°C/min, and the reaction was carried out at a temperature of about 300 to 400°C, so that the product was PCF(AtF3)y (in the formula,
PC is A? 5. The method according to claim 4, characterized in that the carbon is a carbonaceous material. (8) When the graphite raw material is parent irolytic graphite, the mixture is heated under a fluorine atmosphere for about 20 to 10 min.
After holding at a temperature of 0°C for at least about 1 hour, about 2°C ~)
Raise the temperature at a heating rate of ~10°C/min to approximately 300-400°C
The product is PGF(A-/-F5)y
5. The method according to claim 4, wherein PG is .