JPH05208136A - Catalyst for producing nitrile from alkane - Google Patents

Abstract

PURPOSE:To obtain a catalyst for producing nitrile from alkane in high yield by showing an X-ray diffraction peak represented by specific empirical formula at a specific angle of diffraction in an X-ray diffraction line. CONSTITUTION:A catalyst is obtained so that an empirical formula is represented by formula I (wherein X is one or more kind of an element selected from Nb, Ce and the like and, when (a) is l,(b) is 0.01-l.0, (c) is 0.01-1.0 and (x) is 0.01-1.0 and (n) is determined according to the oxidation state of other element) and a condition showing an X-ray diffraction peak at angles 2theta of diffractions (22.1+ or -0.3 deg., 28.2+ or -0.3 deg., 36.2+ or -0.3 deg., 45.2+ or -0.3 deg., 50.0+ or -0,3 deg.) in an X-ray diffraction line is satisfied. By using this catalyst being novel oxide, nitrile can be produced from alkane being a raw material in high yield at relatively low temp. of about 400-459 deg.C without allowing halide or water to be present in a reactional system.

Description

Detailed Description of the Invention

[0001]

FIELD OF THE INVENTION The present invention relates to a method for producing nitrile. More particularly, it relates to an improved nitrile production method using alkane as a raw material.

[0002]

BACKGROUND OF THE INVENTION Nitriles such as acrylonitrile and methacrylonitrile are industrially produced as important intermediates for fibers, synthetic resins, synthetic rubbers and the like. The most general method is to react an olefin such as the above with an ammonia and oxygen in the presence of a catalyst in a gas phase at a high temperature.

On the other hand, due to the price difference between propane and propylene or the price difference between isobutane and isobutene, lower alkanes such as propane and isobutane are used as starting materials, and ammonia and oxygen are used in the presence of a catalyst. There is an increasing interest in the development of a method for producing acrylonitrile and methacrylonitrile by a so-called ammoxidation reaction method in which they are catalytically reacted with each other in the gas phase.

As an example of these reports, Mo-Bi-P
-O catalyst (Japanese Patent Laid-Open No. 48-16887), V-Sb-
O-based catalyst (JP-A-47-33783, JP-B-50-2)
No. 3016, JP-A-1-268668), Sb-U-
V-Ni-O catalyst (Japanese Patent Publication No. 47-14371), S
b-Sn-O type catalyst (Japanese Patent Publication No. 50-28940), V
-Sb-W-P-O catalyst (Japanese Patent Laid-Open No. 95439/1990)
No.), V-Sb-W-O-based oxide and Bi-Ce-Mo-
A catalyst obtained by mechanically mixing W—O type oxides (Japanese Patent Application Laid-Open No. Sho 6-96).
4-38051) and the present inventors
o-V-Te-Nb-O based catalyst (JP-A-2-257)
Is reported.

[0005]

However, none of these methods can sufficiently satisfy the target yield of nitriles. Further, in order to improve the yield of nitriles, a method of adding a small amount of an organic halide, an inorganic halide, or a sulfur compound to the reaction system, or a method of adding water has been tried, but the former is There is a problem of corrosion of the reactor, and the latter has problems such as generation of by-products due to side reactions and treatment thereof, and both of them have problems in industrial implementation.

Further, the conventional method using a catalyst system generally requires an extremely high reaction temperature of about 500 ° C. or higher except for the Mo-V-Te-Nb-O catalyst reported by the present inventors. Therefore, it is not advantageous in terms of reactor material, manufacturing cost, and the like.

[0007]

Means for Solving the Problems As a result of various studies on the production method of nitrile using alkane as a raw material, the present inventors have found that molybdenum (Mo), vanadium (V), tellurium (Te) having a specific crystal structure. In the presence of a catalyst composed of a certain kind of metal, by reacting an alkane with ammonia in a gas phase, a halide and water are not present in the reaction system, and the temperature is relatively low at about 400 to 450 ° C. The present inventors have found that the target nitrile can be produced at a temperature in a significantly higher yield than the conventional method, and have reached the present invention.

The present invention will be described in detail below. The characteristics of the catalyst for producing a nitrile by subjecting an alkane to a gas phase catalytic oxidation reaction of ammonia of the present invention are due to the following points. Empirical formula of the _{catalyst, Mo a V b Te c X} x O in _n (1) (Formula (1), X is Nb, Ta, W, Ti, A
1, Zr, Cr, Mn, Fe, Ru, Co, Rh, N
represents one or more elements selected from i, Pd, Pt, Sb, Bi and Ce, and when a = 1, b = 0.01 to 1.0 c = 0.01 to 1 0.0x = 0.01 to 1.0, and n is determined by the oxidation states of other elements. ). In the X-ray diffraction line of the catalyst, the diffraction angle 2θ shown below
Shows the X-ray diffraction peak.

[0009]

[Table 3] Diffraction angle 2θ (°) 22.1 ± 0.3 28.2 ± 0.3 36.2 ± 0.3 45.2 ± 0.3 50.0 ± 0.3

The catalyst of the present invention is the oxide of the above formula (1), and the above element is used as X, preferably Nb, Ta, W and Ti, and particularly preferably Nb. Further, as a coefficient of the equation (1), when a = 1, b = 0.1 to 0.6, c = 0.05 to 0.4, x =
0.01 to 0.6 is particularly preferable. However, the oxide is not sufficient as the reaction catalyst of the present invention merely by showing the composition of the formula (1), and it is important that the oxide has a specific crystal structure.

An index indicating that the oxide used as the catalyst of the present invention has a specific crystal structure is a powder X-ray diffraction pattern. X-ray diffraction peak of the oxide (C as an X-ray source
u-Kα line) and the specific diffraction angle 2θ
In, there are five major diffraction peaks shown below.

[0012]

[Table 4] X-ray grating plane diffraction angle 2θ (°) Interval median value (Å) Relative intensity 22.1 ± 0.3 4.02 100 28.2 ± 0.3 3.16 20 to 150 36.2 ± 0.3 2.48 5-60 45.2 ± 0.3 2.00 2-40 50.0 ± 0.3 1.82 2-40

The X-ray diffraction peak intensity may deviate depending on the measurement conditions of each crystal, but the relative intensity is usually in the above range when the peak intensity at 2θ = 22.1 ° is 100. Also, in general, 2θ = 22.1 ° and 28.2.
The peak intensity at ° appears significantly. However, as long as the above-mentioned 5 diffraction peaks are recognized, even if there is a peak having a peak at 2θ other than the 5 diffraction peaks, the basic crystal structure does not change and it can be preferably used in the present invention.

The method for preparing the oxide having this specific crystal structure is as follows. For example, Mo _a V _b Te _c Nb
For _x O _n, to an aqueous solution containing a predetermined amount of ammonium metavanadate salt, an aqueous solution of telluric acid, the proportion atomic ratio of metal elements of each of the aqueous solutions of ammonium niobium oxalate salt and ammonium paramolybdate salt is given Are sequentially added in such an amount ratio that they become, and are dried by an evaporation dryness method, a spray drying method, a vacuum drying method, etc. Finally, the remaining dried product is calcined to obtain the target oxide. Further, in order to perform the firing efficiently, the dried product is usually treated in air or an inert gas atmosphere such as nitrogen or argon before the final firing.
You may heat-decompose at 50-350 degreeC.

The calcination conditions of the method for preparing the particular oxide used as the catalyst of the present invention are of particular importance. The firing treatment in the case of preparing an ordinary oxide is most commonly performed in an oxygen atmosphere. However, in the present invention,
It is preferable to set the firing atmosphere substantially in the absence of oxygen, for example, in an atmosphere of an inert gas such as nitrogen, argon or helium, or in the gas, a reducing gas such as hydrogen or hydrocarbon, or steam. Or in vacuum usually 350-700 ° C., preferably 4
It is carried out at a temperature of 00 to 650 ° C for usually 0.5 to 30 hours, preferably 1 to 10 hours. At a temperature lower than the temperature range, formation of the crystal structure having high catalytic activity is insufficient, and at a temperature higher than the temperature range, a part of the crystal structure may be thermally decomposed, which is not preferable.

The oxygen content of the oxide thus obtained
When examining the content, for example, Mo _aV_bTe_cNb_x
O_nIn the case of, the value of n is Mo, V, Te, Nb
Is the value corresponding to the highest oxidation state of (3a + 2.5b +
3c + 2.5x), which is 80 to 97%.
It was That is, of the specific structure used as the catalyst of the present invention
Oxide is the same raw material dried product baked in a normal oxygen atmosphere
It has a slightly lower oxygen content than the oxide obtained by
Nothing more.

Therefore, it is totally unexpected that the oxide not only has a specific crystal structure but also exhibits a significantly superior activity as compared with conventional catalysts in the reaction of nitrile using an alkane as a raw material. It is amazing. The raw materials of the above oxides are not limited to those described above, but instead of ammonium metavanadate, for example, V ₂ O ₅ , V ₂ O ₃ , VOCl ₃ or V may be used.
Cl ₄ or the like can be used, and T can be used in place of telluric acid.
eO ₂ or the like is used, NbCl ₅ , Nb ₂ O ₅ , niobate, or the like is used instead of niobium ammonium oxalate, and M is used instead of ammonium paramolybdate.
oO ₃ , MoCl ₅ , etc. can be used.

The above catalysts can be used alone, but can also be used together with well-known carriers such as silica, alumina, titania, aluminosilicate and diatomaceous earth.
Further, it is molded into an appropriate shape and particle size depending on the scale of reaction, method and the like. In the present invention, a nitrile can be efficiently produced by subjecting an alkane to a gas-phase catalytic oxidation reaction with ammonia in the presence of the above-mentioned catalyst.

The alkane as a raw material in the nitrile production method of the present invention is not particularly limited, and examples thereof include methane, ethane, propane, butane, isobutane,
Pentane, hexane, heptane, cyclohexane and the like can be mentioned, but considering the industrial use of the resulting nitrile, it is preferable to use a lower alkane having 1 to 4 carbon atoms, particularly propane and isobutane.

Although the details of the mechanism of the oxidation reaction in the present invention are not clear, it is carried out by oxygen atoms present in the above oxides or molecular oxygen present in the feed gas. When the molecular oxygen is present in the feed gas, the molecular oxygen may be pure oxygen gas, but it is generally economical to use an oxygen-containing gas such as air because purity is not particularly required. Alkane, a mixed gas of ammonia and an oxygen-containing gas is usually used as the supply gas, but a mixed gas of an alkane and ammonia and an oxygen-containing gas may be alternately supplied.

It is also possible to carry out a gas phase catalytic reaction using only alkane and ammonia, which are substantially free of molecular oxygen, as feed gases. In such a case, a method is preferable in which a part of the catalyst is appropriately extracted from the reaction zone, the catalyst is sent to an oxidation regenerator, and after regeneration, the catalyst is re-supplied to the reaction zone. Examples of the method for regenerating the catalyst include a method in which an oxidizing gas such as oxygen, air or nitric oxide is passed through the catalyst in the regenerator usually at 300 to 600 ° C.

In the case of using propane as the alkane and air as the oxygen source, the ratio of the air supplied to the reaction is important with respect to the selectivity of the acrylonitrile produced, and the air is Usually, the acrylonitrile selectivity is high in a range of 25 mol times or less, particularly 1 to 15 mol based on propane. Further, the proportion of ammonia supplied to the reaction is preferably in the range of 0.2 to 5 mol times, and particularly 0.5 to 3 mol times the amount of propane. The reaction is usually carried out under atmospheric pressure, but it can also be carried out under slightly elevated pressure or reduced pressure. For other alkanes, the composition of the feed gas is selected according to the reaction conditions for propane.

In the method of the present invention, a temperature lower than that in the conventional ammoxidation reaction of alkane, for example, 34
It can be carried out at 0 to 480 ° C, and particularly preferably about 400 to 450 ° C. The gas space velocity SV in the gas phase reaction is usually 100～10000H ^-1, preferably in the range of 300~2000h ^-1. In addition,
As a diluent gas for adjusting the space velocity and oxygen partial pressure,
An inert gas such as nitrogen, argon or helium can be used. When the ammoxidation reaction of propane is carried out by the method of the present invention, carbon monoxide, carbon dioxide, acetonitrile, hydrocyanic acid, acrolein, etc. are by-produced in addition to acrylonitrile, but the amount produced is extremely small.

[0024]

EXAMPLES The present invention will be described in more detail below with reference to Examples and Comparative Examples, but the present invention is not limited to these Examples as long as the gist thereof is not exceeded. The conversion rate (%) in the following examples and comparative examples,
The selectivity (%) and the yield (%) are respectively shown by the following equations.

[0025]

[Formula 1] Alkane conversion rate (%) = (mol number of consumed alkane / mol number of supplied alkane) × 100 Selectivity of target nitrile (%) = (mol number of target nitrile to be produced / mol number of consumed alkane) × 100 Yield of target nitrile (%) = (mol number of nitrile for production / mol number of alkane supplied) × 100

Example 1 Experimental An oxide having the composition Mo ₁ V _0.4 Te _0.2 Nb _0.1 O _n was prepared as follows. 4.21 in 117 ml of warm water
g of ammonium metavanadate is dissolved, and 4.13 g of telluric acid and ammonium paramolybdate 1 are dissolved therein.
5.89 g was sequentially added to prepare a uniform aqueous solution. Further, add 3.99 g of niobium ammonium oxalate salt to 1
A liquid dissolved in 7.9 ml of water was mixed to prepare a slurry. This slurry was evaporated to dryness at about 150 ° C. to obtain a dried product.

5 mm of this dried product was obtained using a tablet molding machine.
After being molded into φ × 3 mmL, it was pulverized, sieved to 16 to 28 mesh, and fired at 620 ° C. for 2 hours in a nitrogen stream.
The powder X-ray diffraction line peak chart of the oxide thus obtained is shown in FIG. 1, and the main diffraction line peak intensity thereof is shown in Table-1. The oxygen content in the oxide was measured by an oxygen analyzer and found to be 31.0% by weight. The coefficient n of O (oxygen) calculated from this measured value is 4.25. n = 4.25 means that the highest oxidation state of the constituent elements of the oxide is Mo = 6, V = 5, Te = 6, and Nb = 5.
Since n = 4.85 when the valence is set, 8
This corresponds to 7.6%.

0.5 ml of the catalyst thus obtained was charged into a reactor, the reaction temperature was 440 ° C., and the space velocity SV was 100.
Fixed at ⁰ h ^-1 , propane: ammonia: air = 1:
Gas was supplied at a molar ratio of 1.2: 10 to carry out a gas phase catalytic reaction. The results are shown in Table-2.

Examples 2 and 3 Experimental composition Mo ₁ V _0.4 Te _0.2 N was carried out in the same manner as in Example 1 except that the firing temperature was changed to 500 ° C. and 600 ° C.
an oxide having a b _0.1 O _n was prepared. The results of powder X-ray diffraction of the oxide are shown in Table 1. Table 2 shows the results of the gas phase contact reaction.

Comparative Example 1 An oxide having the experimental composition Mo ₁ V _0.4 Te _0.2 O _n was obtained in the same manner as in Example 2 except that the niobium component was not used in Example 2. The X-ray diffraction pattern of the oxide was quite different from that of Example 1. Table 2 shows the results of the gas phase contact reaction.

Comparative Example 2 Experimental composition Mo ₁ V _0.4 Te _0.2 was carried out in the same manner as in Example 1 except that firing was carried out at 350 ° C. for 2 hours under air flow.
An oxide having a nb _0.1 O _n was prepared. The powder X-ray diffraction pattern of the obtained oxide is shown in FIG. The pattern is completely different from that of FIG. 1 of the first embodiment. Table 2 shows the results of the gas phase contact reaction.

Comparative Examples 3 and 4 Using the oxide of Comparative Example 2, a gas phase catalytic reaction was carried out under the reaction conditions shown in Table 2. The results are shown in Table-2.

Example 4 Experimental An oxide having the composition Mo ₁ V _0.4 Te _0.2 Sb _0.1 O _n was prepared as follows. 4.21 in 117 ml of warm water
g of ammonium metavanadate is dissolved, and 4.13 g of telluric acid and ammonium paramolybdate 1 are dissolved therein.
5.9 g was sequentially added to prepare a uniform aqueous solution. To this, 1.56 g of antimony chloride oxide was dissolved in 17.9 ml of water and mixed. The obtained aqueous solution was evaporated to dryness to obtain a dried product. 5 mmφ of this dried product using a tablet press
After molding into 3 mmL, it was crushed, sieved to 16 to 28 mesh, and fired at 500 ° C. for 2 hours in a nitrogen stream. The results of powder X-ray diffraction of the obtained oxide are shown in Table 1. Table 2 shows the results of the gas phase contact reaction of the oxides thus obtained.

Comparative Example 5 Mo ₁ V _0.4 Te _0.2 Sb _0.1 was carried out in the same manner as in Example 4 except that calcination was carried out in air at 350 ° C. for 2 hours.
An oxide having O _n was prepared. The X-ray diffraction pattern of the resulting oxide was quite different from that of Example 4.
In addition, Table 2 shows the results of a gas phase catalytic reaction using the obtained oxide.

Example 5 An oxide was prepared in the same manner as in Example 4 except that 3.38 g of aluminum nitrate nonahydrate was used in place of the antimony chloride oxide in Example 4. Empirical composition of the obtained oxide is _{Mo 1 V 0.4 Te 0.2 Al 0.1} O n. The results of powder X-ray diffraction of the oxide thus obtained are shown in Table 1. In addition, Table 2 shows the results of a gas phase catalytic reaction using the obtained oxide.

Comparative Example 6 Mo ₁ V _0.4 Te _0.2 Al _0.1 was carried out in the same manner as in Example 5 except that firing was carried out at 350 ° C. for 2 hours under air flow in Example 5.
An oxide having O _n was prepared. The X-ray diffraction pattern of the resulting oxide was completely different from that of Example 5. In addition, Table 2 shows the results of a gas phase catalytic reaction using the obtained oxide.

Example 6 0.415 g of palladium nitrate was used in place of the antimony chloride oxide in Example 4, and the firing temperature was 600.
An oxide was prepared in the same manner as in Example 4 except that the temperature was changed to ° C. The experimental composition of the obtained oxide was Mo ₁ V _0.4 Te _0.2 Nb.
A _0.1 Pd _0.02 O _n. The results of powder X-ray diffraction of the oxide thus obtained are shown in Table 1. In addition, Table 2 shows the results of a gas phase catalytic reaction using the obtained oxide.

Examples 7 to 23 Oxides of each experimental composition were prepared in the same manner as in Example 1 except that the ratio of the raw material compounds was changed by the method of Example 1 and the firing temperature was set to 600 ° C. Prepared. Powder of each oxide X
The results of the line diffraction are shown in Table-1. In addition, Table 3 shows the results of the gas phase contact reaction using each oxide.

Examples 24-32 Oxides prepared in Example 3 (experimental composition Mo ₁ V _0.4 Te
The results of the gas-phase catalytic oxidation reaction under various conditions using the _0.2 Nb _0.1 O _n) shown in Table 4.

[0040]

[Table 5]

[0041]

[Table 6]

[0042]

[Table 7]

[0043]

[Table 8]

Example 33 Experimental An oxide having the composition Mo ₁ V _0.3 Te _0.23 Nb _0.12 O _n was prepared as follows. Dissolve 15.7 g of ammonium metavanadate in 325 ml of warm water,
To this, 23.6 g of telluric acid and 78.9 g of ammonium paramolybdate were sequentially added to prepare a uniform aqueous solution. Further, 117.5 g of an aqueous solution of ammonium niobium oxalate having a niobium concentration of 0.456 mol / kg is mixed,
A slurry was prepared. The slurry was evaporated to dryness to give a solid. 5 mmφ x 3 of this solid using a tablet press
After molding into mmL, it was pulverized, sieved to 16 to 28 mesh, and fired at 600 ° C for 2 hours in a nitrogen stream.

When the powder X-ray diffraction measurement of the oxide thus obtained was carried out (using Cu-Kα ray), the diffraction angles 2θ (°) were 22.1 (100), 28.2 (9).
0.0), 36.2 (25.7), 45.1 (15.
2) A major diffraction peak was observed at 50.0 (16.3) (numbers in parentheses indicate a peak at 22.1 ° of 100).
Indicates the relative peak intensity. ).

0.5 ml of the catalyst thus obtained was charged into a reactor and the reaction temperature was 420 ° C. and the space velocity SV was 100.
Fixed at 0h ^-1 , isobutane: ammonia: air =
Gas was supplied at a molar ratio of 1: 1.2: 15 to carry out a gas phase catalytic reaction. As a result, the conversion rate of isobutane was 61.
4%, the selectivity of methacrylonitrile was 29.7%, and the yield of methacrylonitrile was 19.1%.

Example 34 A gas phase catalytic oxidation reaction of isobutane was carried out in the same manner as in Example 33 except that the oxide of Example 3 was used. As a result, the conversion of isobutane was 52.1%, the selectivity of methacrylonitrile was 31.0%, and the yield of methacrylonitrile was 16.
It was 2%.

Comparative Example 7 A vapor phase catalytic oxidation reaction of isobutane was carried out in the same manner as in Example 33 except that the oxide of Comparative Example 2 was used. As a result, the conversion rate of isobutane was 11.0%, the selectivity of methacrylonitrile was 42.7%, and the yield of methacrylonitrile was 4.7.
%Met.

Example 35 Experimental composition A material in which silica accounts for 10 wt% of the oxide having Mo ₁ V _0.3 Te _0.23 Nb _0.12 O _n was prepared as follows. 3.79 g of ammonium metavanadate was dissolved in 117 ml of warm water, and 3.72 g of telluric acid and ammonium paramolybdate 14.3 were dissolved in the solution.
0 g was sequentially added to prepare a uniform aqueous solution. Furthermore, 3.59 g of niobium ammonium oxalate salt was added to 17.9 ml.
Liquid dissolved in water, silica sol (silica content 20 wt
%) 10.24 g was mixed to prepare a slurry. This slurry was evaporated to dryness at 150 ° C. to obtain a dried product.

5 mm of this dried product was obtained using a tablet molding machine.
After being molded into φ × 3 mmL, it was crushed, sieved to 16 to 28 mesh, and fired at 600 ° C. for 4 hours in a nitrogen stream.
The powder X-ray diffraction measurement of the thus-obtained oxide was carried out and found to be 22.1 (10) as a diffraction angle 2θ (°).
0), 28.2 (41.7), 36.2 (10.0),
Major diffraction peaks were observed at 45.2 (13.1) and 50.0 (7.1) (the numbers in parentheses indicate relative peak intensities when the peak at 22.1 ° C. is 100). ).

0.5 ml of the substance thus obtained was charged into a reactor and the reaction temperature was 420 ° C. and the space velocity SV was 100.
Fixed at ⁰ h ^-1 , propane: ammonia: air = 1:
Gas was supplied at a molar ratio of 1.2: 15 to carry out a gas phase catalytic oxidation reaction. As a result, the conversion rate of propane was 88.9.
%, The acrylonitrile selectivity was 60.5%, and the acrylonitrile yield was 53.8%.

[0052]

EFFECTS OF THE INVENTION According to the method of the present invention, the use of a novel oxide from an alkane as a raw material allows the reaction system to have a temperature of 400-400 without the presence of halide or water.
The target nitrile can be produced in a high yield at a relatively low temperature of about 450 ° C.

[Brief description of drawings]

1 shows a powder X-ray diffraction pattern of the oxide of Example 1. FIG.

FIG. 2 shows a powder X-ray diffraction pattern of the oxide of Comparative Example 2.

 ─────────────────────────────────────────────────── ─── Continuation of front page (72) Inventor Tomoaki Umezawa 1 Toho-cho, Yokkaichi-shi, Mie Mitsubishi Kasei Co., Ltd. Yokkaichi Plant

Claims (4)

[Claims] 1. A catalyst for producing a nitrile from an alkane satisfying the following conditions: Empirical formula of the _{catalyst, Mo a V b Te c X} x O in _n (1) (Formula (1), X is Nb, Ta, W, Ti, A
1, Zr, Cr, Mn, Fe, Ru, Co, Rh, N
represents one or more elements selected from i, Pd, Pt, Sb, Bi and Ce, and when a = 1, b = 0.01 to 1.0 c = 0.01 to 1 0.0x = 0.01 to 1.0, and n is determined by the oxidation states of other elements. ). In the X-ray diffraction line of the catalyst, the diffraction angle 2θ shown below
Shows the X-ray diffraction peak. [Table 1] Diffraction angle 2θ (°) 22.1 ± 0.3 28.2 ± 0.3 36.2 ± 0.3 45.2 ± 0.3 50.0 ± 0.3 2. A compound of molybdenum, vanadium and tellurium, and niobium, tantalum, tungsten, titanium,
Aluminum, zirconium, chromium, manganese, iron,
An aqueous solution containing a compound of one or more elements selected from ruthenium, cobalt, rhodium, nickel, palladium, platinum, antimony, bismuth and cerium is dried, and the remaining dried product is obtained in the absence of oxygen. The method for producing the catalyst according to claim 1, wherein the catalyst is calcined. 3. A process for producing a nitrile, which comprises subjecting an alkane to a gas phase catalytic oxidation reaction with ammonia in the presence of a catalyst satisfying the following conditions: Empirical formula of the _{catalyst, Mo a V b Te c X} x O in _n (1) (Formula (1), X is Nb, Ta, W, Ti, A
1, Zr, Cr, Mn, Fe, Ru, Co, Rh, N
represents one or more elements selected from i, Pd, Pt, Sb, Bi and Ce, and when a = 1, b = 0.01 to 1.0 c = 0.01 to 1 0.0x = 0.01 to 1.0, and n is determined by the oxidation states of other elements. ). In the X-ray diffraction line of the catalyst, the diffraction angle 2θ shown below
Shows the X-ray diffraction peak. [Table 2] Diffraction angle 2θ (°) 22.1 ± 0.3 28.2 ± 0.3 36.2 ± 0.3 45.2 ± 0.3 50.0 ± 0.3 4. A compound of molybdenum, vanadium and tellurium with niobium, tantalum, tungsten, titanium,
Aluminum, zirconium, chromium, manganese, iron,
An aqueous solution containing a compound of one or more elements selected from ruthenium, cobalt, rhodium, nickel, palladium, platinum, antimony, bismuth and cerium is dried, and the remaining dried product is obtained in the absence of oxygen. A process for producing a nitrile, which comprises subjecting ammonia to a gas-phase catalytic oxidation reaction in the presence of a catalyst that satisfies the following conditions obtained by calcination. Empirical formula of the _{catalyst, Mo a V b Te c X} x O in _n (1) (Formula (1), X is Nb, Ta, W, Ti, A
1, Zr, Cr, Mn, Fe, Ru, Co, Rh, N
represents one or more elements selected from i, Pd, Pt, Sb, Bi and Ce, and when a = 1, b = 0.01 to 1.0 c = 0.01 to 1 0.0x = 0.01 to 1.0, and n is determined by the oxidation states of other elements. ).