JP7109254B2 - Reactor and method for producing olefin - Google Patents

Description

The present disclosure relates to reactors and processes for producing olefins.

BACKGROUND ART Techniques for producing olefins by Oxidative Coupling of Methane (hereinafter referred to as OCM reaction) using a gas containing methane such as natural gas are known. Patent Document 1 describes the production of olefin by introducing methane, water vapor, and oxygen from the same position in the direction of gas flow into an OCM reaction catalyst (OCM catalyst) (especially see FIG. 2). It also describes that hydrocarbons having 2 or more carbon atoms are supplied outside the OCM catalyst and downstream of the gas flow.

U.S. Patent Application Publication No. 2016/0237003

By the way, the present inventors have studied and found that the technique described in Patent Document 1 still has room for improvement in the olefin selectivity. In other words, it was found that the technique described in Patent Document 1 still produces a large amount of carbon oxides such as carbon dioxide by-products, and can further increase the selectivity of olefins such as ethylene.

An object of at least one embodiment of the present disclosure is to provide a reactor capable of improving the selectivity of olefins and a method for producing olefins.

(1) A reactor according to an embodiment of the present disclosure,
A reactor for producing olefins from a first gas containing methane using a partial oxidation coupling catalyst,
a housing;
a catalyst container disposed inside the housing, the catalyst container having therein a catalyst layer composed of the partial oxidation coupling catalyst;
a first gas introduction passage for introducing the first gas from the outside of the housing into the interior of the catalyst container through a first introduction portion formed in the catalyst container;
Vapor and oxygen are introduced into the catalyst container from the outside of the housing through a second introduction portion formed in the catalyst container at a position different from the first introduction portion. a second gas introduction channel for introducing a second gas containing
with
The first gas and the second gas are separately introduced into the catalyst container .

According to the above (1), hydroxyl radicals can be generated from the water vapor and oxygen introduced from the second inlet. As a result, the generated hydroxyl radical is used to activate methane as a methyl radical, the methyl radical is coupled to generate ethane, and the dehydrogenation reaction can generate ethylene, resulting in a higher olefin selectivity than before. can be improved.

(2) In some embodiments, in the configuration of (1) above,
The catalyst container is formed with a discharge part for discharging the olefin produced in the catalyst layer,
The first introduction section is arranged so as to join the first gas with a gas flow from the second introduction section toward the discharge section.

According to (2) above, the first gas containing methane can join the hydroxyl radicals generated from the water vapor and oxygen introduced from the second inlet. This makes it possible to generate methyl radicals from the generated hydroxy radicals and methane, thereby facilitating the generation of ethane and ethylene.

(3) In some embodiments, in the configuration of (1) or (2) above,
one of the first gas introduction channel and the second gas introduction channel is formed by an internal space defined between the inner surface of the housing and the outer surface of the catalyst container;
The other of the first gas introduction channel and the second gas introduction channel is formed inside an introduction pipe extending in the internal space from the inner surface of the housing to the outer surface of the catalyst container. It is characterized by being

According to (3) above, the gas introduced into the internal space can be easily distributed throughout the catalyst layer. As a result, local reactions can be suppressed, and uneven reaction in the catalyst layer can be suppressed.

(4) In some embodiments, in the configuration of (3) above,
the second gas introduction channel is formed by an internal space defined between the inner surface of the housing and the outer surface of the catalyst container;
The first gas introduction channel is formed inside an introduction pipe extending in the internal space from the inner surface of the housing to the outer surface of the catalyst container.

According to (4) above, the second gas containing water vapor and oxygen can be easily spread over the entire catalyst layer. As a result, it is possible to easily generate hydroxyl radicals having high reactivity in the entire catalyst layer, and to facilitate reaction with methane in the entire catalyst layer.

(5) In some embodiments, in the configuration of (3) or (4) above,
The catalyst container is formed with a discharge part for discharging the olefin produced in the catalyst layer,
The catalyst container includes a first wall surface, a second wall surface facing the first wall surface, and a side wall surface connecting the first wall surface and the second wall surface,
The first introduction portion is formed on the first wall surface,
The second introduction portion is formed on the side wall surface,
The discharge part is formed on the second wall surface.

According to (5) above, in the catalyst layer, the gas can come into contact with the gas flowing from the first wall surface to the second wall surface from the side. Thereby, the contact between the first gas and the second gas can be promoted, and the production of olefin can be promoted.

(6) In some embodiments, in the configuration of (3) or (4) above,
The catalyst container is formed with a discharge part for discharging the olefin produced in the catalyst layer,
The catalyst container is
a first wall surface;
a second wall surface formed at a position facing the first wall surface;
a side wall surface connecting the first wall surface and the second wall surface;
a discharge channel for discharging the olefin produced in the catalyst layer, the discharge channel extending between a first wall surface and a second wall surface and connecting to the discharge part; including a discharge channel forming member,
The first introduction part and the discharge part are formed on the first wall surface,
The second introducing portion is formed on the side wall surface.

According to (6) above, the heat of the olefin produced in the catalyst layer can be applied to the catalyst layer. Thereby, the catalyst layer can be heated.

(7) In some embodiments, in the configuration of (5) or (6) above,
The first gas introduction channel is
a first gas introduction main flow path for introducing the first gas from the outside of the housing into the interior of the catalyst container through a first main introduction portion formed on the first wall surface of the catalyst container;
a first gas introduction sub-flow path for introducing the first gas from the outside of the housing into the interior of the catalyst container through a first sub-introduction portion formed on the side wall surface of the catalyst container; characterized by comprising

According to (7) above, the first gas containing methane can be introduced into the catalyst layer at a plurality of locations. Thereby, reaction unevenness in the catalyst layer can be suppressed.

(8) In some embodiments, in the configuration of any one of (1) to (7) above,
The reactor further includes a heating pipe through which a heating gas flows, which is arranged so as to penetrate the catalyst layer.

According to (8) above, the catalyst layer can be heated by the heating gas. Thereby, the production amount of olefin can be increased.

(9) In some embodiments, in the configuration of any one of (1) to (8) above,
The partial oxidation coupling catalyst is characterized by containing an alkali metal.

According to the above configuration (9), an alkali metal oxide and hydrogen peroxide can be produced as intermediates, making it easier to produce hydroxyl radicals.

(10) In some embodiments, in the configuration of any one of (1) to (9) above,
the second gas includes methane;
In the second gas, the molar ratio of methane to oxygen contained in the second gas is 0.01 or more and 0.05 or less.

According to the configuration (10) above, the auxiliary supplied methane can be burned to quickly raise the temperature of the catalyst layer. Thereby, the partial oxidation coupling reaction can be promoted and the catalytic efficiency can be improved.

(11) A method for producing an olefin according to an embodiment of the present disclosure,
A method for producing an olefin from a first gas containing methane using a partial oxidation coupling catalyst, comprising:
The first gas or the second gas containing water vapor and oxygen is supplied to a catalyst container arranged inside a housing, the catalyst container having a catalyst layer composed of the partial oxidation coupling catalyst inside. a first introduction step of introducing one of the gases;
a second introduction step of introducing the other of the first gas and the second gas into the catalyst container at a position different from the introduction part of the one gas;
including
The first gas and the second gas are separately introduced into the catalyst container .

According to the configuration (11) above, it is possible to generate hydroxyl radicals from water vapor and oxygen contained in the second gas. As a result, ethylene can be produced using the produced hydroxy radicals, and the olefin selectivity can be improved more than before.

ADVANTAGE OF THE INVENTION According to at least one embodiment of this invention, the reactor which can improve the selectivity of an olefin more than before, and the manufacturing method of an olefin can be provided.

It is a sectional view of a reactor concerning a 1st embodiment of the present invention. It is a figure explaining the reaction flow performed in sectional drawing shown in FIG. FIG. 4 is a cross-sectional view of a reactor according to a second embodiment of the invention; FIG. 4 is a cross-sectional view taken along the line AA in FIG. 3; FIG. 5 is a cross-sectional view of a reactor according to a third embodiment of the invention; FIG. 6 is a cross-sectional view taken along the line BB in FIG. 5; FIG. 4 is a cross-sectional view of a reactor according to a fourth embodiment of the invention;

Several embodiments of the present invention will now be described with reference to the accompanying drawings. However, the contents described as embodiments or the contents described in the drawings below are merely examples, and can be arbitrarily changed and implemented without departing from the scope of the present invention. Moreover, each embodiment can be implemented by combining two or more arbitrarily. Furthermore, in each embodiment, common members are denoted by the same reference numerals, and overlapping descriptions are omitted for simplification of description.

In addition, the dimensions, materials, shapes, relative arrangements, etc. of components described as embodiments or shown in the drawings are not meant to limit the scope of the present invention, but are merely illustrative examples. do not have.
For example, expressions denoting relative or absolute arrangements such as "in a direction", "along a direction", "parallel", "perpendicular", "center", "concentric" or "coaxial" are strictly not only represents such an arrangement, but also represents a state of relative displacement with a tolerance or an angle or distance to the extent that the same function can be obtained.
For example, expressions such as "identical", "equal", and "homogeneous", which express that things are in the same state, not only express the state of being strictly equal, but also have tolerances or differences to the extent that the same function can be obtained. It shall also represent the existing state.
For example, expressions that express shapes such as squares and cylinders do not only represent shapes such as squares and cylinders in a geometrically strict sense, but also include irregularities and chamfers to the extent that the same effect can be obtained. The shape including the part etc. shall also be represented.
On the other hand, the expressions "comprising", "comprising", "having", "including", or "having" one component are not exclusive expressions excluding the presence of other components.

FIG. 1 is a cross-sectional view of a reactor 100 according to a first embodiment of the invention. Reactor 100 is for producing olefins from a first gas containing methane using a partial oxidation coupling catalyst (OCM catalyst). The reactor 100 includes a housing 1 , a catalyst container 25 , a first gas introduction channel 32 and a second gas introduction channel 33 .

Among these, the catalyst container 25 is arranged inside the housing 1 and has a catalyst layer 21 made of an OCM catalyst inside. The catalyst container 25 is supported by the housing 1 by a support member (not shown). The catalyst layer 21 is configured, for example, in a cylindrical shape.

Any OCM catalyst can be used as long as it can produce an olefin by a partial oxidation coupling reaction of methane, but the OCM catalyst preferably contains an alkali metal. By using an OCM catalyst containing an alkali metal, an oxide of an alkali metal and hydrogen peroxide can be produced as intermediates, facilitating the production of hydroxyl radicals (described below). Alkali metals include, for example, sodium, potassium, lithium, etc. Among them, sodium and potassium are preferred, and sodium is particularly preferred. Specific examples of OCM catalysts include, for example, Mn/Na ₂ WO ₄ /SiO ₂ catalysts. Also, the reaction temperature of the OCM reaction can be, for example, 800.degree. C. to 1100.degree.

Also, the catalyst container 25 is formed with a discharge part 27 for discharging the olefin produced in the catalyst layer 21 . The catalyst container 25 includes a first wall surface 22, a second wall surface 23 formed at a position facing the first wall surface 22, and a side wall surface 24 connecting the first wall surface 22 and the second wall surface 23. . Among these, the first wall surface 22 and the second wall surface 23 are flat plates, and the side wall surface 24 is, for example, a perforated plate formed in an annular shape. Therefore, the catalyst container 25 is formed in a cylindrical shape with closed upper and lower surfaces and holes in the side wall surfaces.

The first gas introduction passage 32 is for introducing the first gas from the outside of the housing 1 into the catalyst container 25 via the first introduction portion 26 formed on the first wall surface 22 of the catalyst container 25 . It is. The first introduction part 26 is, for example, a perforated plate. The first gas introduction channel 32 extends from the inner surface of the housing 1 to the outer surface of the catalyst container 25 and extends within the internal space 31 defined between the inner surface of the housing 1 and the outer surface of the catalyst container 25. It is formed inside the introduction tube 11 . The first gas flowing through the first gas introduction channel 32 enters the first gas introduction channel 32 through the supply port 2 . Note that the first gas is, for example, natural gas, methane fermentation gas, or the like. Also, the pressure of the first gas is, for example, greater than 0 MPa, preferably 0.5 MPa or more, and the upper limit is, for example, 1 MPa or less.

The second gas introduction flow path 33 is formed in the side wall surface 24 of the catalyst container 25, and is formed at a position different from the first introduction portion 26. It is for introducing a second gas containing water vapor and oxygen into the catalyst container 25 from the outside of the housing 1 . A second gas introduction channel 33 is formed by the internal space 31 . The second gas flowing through the second gas introduction channel 33 enters the second gas introduction channel 33 through the supply port 3 . The pressure of the second gas is, for example, greater than 0 MPa, preferably 0.5 MPa or more, and the upper limit is, for example, 1 MPa or less.

In this manner, one of the first gas introduction channel 32 and the second gas introduction channel 33 is formed by the internal space 31, and the other is formed inside the introduction pipe 11, so that gas is introduced into the internal space 31. The gas can be easily spread over the entire catalyst layer 21 . As a result, local reactions can be suppressed, and uneven reaction in the catalyst layer 21 can be suppressed. Among them, the second gas introduction channel 33 is formed by the internal space 31 and the first gas introduction channel 32 is formed inside the introduction pipe 11, so that the second gas containing water vapor and oxygen is introduced into the catalyst layer 21. It can be easily distributed throughout. As a result, highly reactive hydroxyl radicals can be easily generated in the entire catalyst layer, and reaction with methane can easily occur in the entire catalyst layer 21 .

The amount of water vapor and oxygen contained in the second gas is not particularly limited. For example, the water vapor concentration contained in the second gas is, for example, 0.01 or more, preferably 0.03 or more, and for example, 0.1 or less, preferably 0, as a molar ratio of water vapor to methane contained in the first gas. 0.07 or less, more preferably 0.05 or less. Furthermore, the oxygen concentration contained in the second gas is, for example, 0.06 or more, preferably 0.08 or more, and for example, 0.5 or less, preferably 0, as a molar ratio of oxygen to methane contained in the first gas. .2 or less.

In addition, the second gas may contain methane as an auxiliary. If supplemental methane is included, it is preferred that the methane content is trace. Specifically, for example, in the second gas, the molar ratio of methane to oxygen contained in the second gas is, for example, 0.01 or more and 0.05 or less. When the methane concentration is within this range, the methane that is supplementarily supplied can be burned and the temperature of the catalyst layer 21 can be quickly raised. Thereby, the OCM reaction can be promoted and the catalytic efficiency can be improved.

Olefins (ethylene, propylene, etc.) produced in the catalyst layer 21 are withdrawn from the reactor 100 through the outlet 27 (formed of, for example, a perforated plate), the outlet pipe 12 and the outlet 4 .

In the catalyst container 25, the first introduction portion 26 is formed on the first wall surface 22, the second introduction portion 28 is formed on the side wall surface 24, and the discharge portion 27 is formed on the second wall surface 23, as described above. By doing so, in the catalyst layer 21, the gas can come into contact with the gas flowing from the first wall surface 22 to the second wall surface 23 from the side. Thereby, the contact between the first gas and the second gas can be promoted, and the production of olefin can be promoted.

In addition, in order to bring the gas into contact with the gas flowing from the first wall surface 22 to the second wall surface 23 from the side, the first introduction part 26 has a , arranged to merge the first gas. By doing so, the first gas containing methane can join the hydroxyl radicals generated from the water vapor and oxygen introduced from the second introduction part 28 . This makes it possible to generate methyl radicals from the generated hydroxy radicals and methane, thereby facilitating the generation of ethane and ethylene.

Although not shown, the catalyst container 25 may be supplied with the first gas from a plurality of portions. That is, the first gas introduction channel 32 may be a plurality of systems, and the first gas introduction channel 32 corresponding to the first gas introduction main channel and the first gas introduction channel 32 corresponding to the first gas introduction sub-channel. It may also include an introduction channel 32 (a plurality of channels may be provided). Both the first gas introduction main flow path and the first gas introduction sub-flow path are connected to the housing 1 via a first introduction portion 26 (first main introduction portion) formed in the first wall surface 22 of the catalyst container 25 . for introducing the first gas into the catalyst container 25 from the outside. By doing so, the first gas containing methane can be introduced into the catalyst layer 21 at a plurality of locations. Thereby, reaction unevenness in the catalyst layer 21 can be suppressed.

According to the reactor 100 described above, hydroxyl radicals can be generated from the steam and oxygen introduced from the second introduction section 28 . As a result, the generated hydroxyl radical is used to activate methane as a methyl radical, the methyl radical is coupled to generate ethane, and the dehydrogenation reaction can generate ethylene, resulting in a higher olefin selectivity than before. can be improved.

In the above example, the first gas is introduced from the supply port 2 and the second gas is introduced from the supply port 3. can be

FIG. 2 is a diagram explaining the flow of reaction performed in the cross-sectional view shown in FIG. This reaction flow is performed in the reactor 100 described above, and is a method for producing olefins from a first gas containing methane using an OCM catalyst. Although FIG. 2 shows that methane is supplied after generation of hydroxyl radicals for the sake of convenience, the first gas and the second gas are supplied to the reactor 100 at the same time.

First, the second gas (or the first gas) is introduced into the catalyst container 25, and water vapor and oxygen react in the catalyst layer 21 (step S1, first introduction step). As a result, hydroxyl radicals are generated (step S2). Next, the first gas is introduced into the catalyst container 25 at a position different from the second introduction part 28, and the introduced methane reacts with the hydroxyl radical. (Step S3, second introduction step). Thereby, methyl radicals are generated (step S4).

Then, the two methyl radicals react (step S5) to produce ethane (step S6). Subsequently, ethylene is produced by a dehydrogenation reaction of ethane produced here (step S7).

The reactions in each of the above steps are outlined by the following elementary reactions. When the catalytically active species is sodium oxide,
_{Na2O + 0.5O2} → _{Na2O2
Na2O2 + H2O} → _{Na2O + H2O2}
H ₂ O ₂ →2OH. (OH. is a hydroxyl radical)
CH ₄ +OH.→CH _3. +H ₂ O (CH3. is a methyl radical)
2CH _3. →C ₂ H _{6
C2H6 → C2H4 + H2}
Each reaction proceeds. Although the description of the reaction formula is omitted, for example, a methyl radical reacts with an alkane (such as ethane) to produce an alkane having one more carbon atom (such as propane). Then, the alkane having one carbon atom is dehydrogenated to produce an olefin (such as propylene).

In addition to these reactions, a side reaction that produces at least one of CO or CO ₂ and a side reaction that produces water can proceed. Namely
CH4+ _2O2- > _{CO2 + 2H2O}
CH4 _{+ 0.5O2} →CO ₊ H2
CO ₊ 0.5O2→ _CO2
H2 _{+ 0.5O2} → _H2O
side reaction can proceed. As the side reactions progress, methane, which is a raw material for producing olefins such as ethylene, is consumed. Therefore, from the viewpoint of increasing the selectivity of olefins, the side reactions are preferably suppressed.

According to the reaction flow described above, hydroxyl radicals can be generated from water vapor and oxygen contained in the second gas. As a result, ethylene can be produced using the produced hydroxy radicals, and the olefin selectivity can be improved more than before.

Here, the present inventors evaluated the olefin selectivity using the reactor 100 described above.

First, as Example 1, the following tests were conducted. A Mn/Na ₂ WO ₄ /SiO ₂ catalyst was used as the OCM catalyst. This catalyst was produced as follows. First, Na ₂ WO ₄ .2H ₂ O (purity 99% by mass), silicic anhydride (Nippon Aerosil Co., Ltd., Aerosil 130) and manganese (purity 99% by mass) were prepared as reagents. These were weighed in equimolar amounts, dissolved in water, stirred and mixed, and water was removed with a rotary evaporator. Then, after heating at 80° C. for 3 hours in an oven, it was further heated in a heating furnace at a heating rate of 120° C./h for 8 hours while circulating dry air (final temperature reached 900° C.). After heating, by cooling to room temperature, a powder of Mn/Na ₂ WO ₄ /SiO ₂ catalyst was produced as an OCM catalyst.

This OCM catalyst is placed in a catalyst container of a test reactor simulating the reactor 100 described above, and a first gas consisting only of methane and a second gas consisting only of water vapor and oxygen are separated from the catalyst container. was introduced into the catalyst layer through the feed port of At this time, the molar ratio of oxygen per unit flow rate to methane was set to 0.05, and the molar ratio of water vapor to methane per unit flow rate was set to 0.04. Then, the inside of the reactor 100 (specifically, the catalyst layer 21) was set to 900° C. to continuously produce olefin.

As a result, the conversion of methane was 18.9%. The ethylene selectivity was 65.4% and the propylene selectivity was 1.0%. Furthermore, the selectivity for carbon monoxide was 8.8% and the selectivity for carbon dioxide was 15.4%. These values are all based on carbon.

Next, as Example 2, the inside of the reactor 100 was set to 1000° C. using a heating device, and the molar ratio of oxygen per unit flow rate to methane was set to 0.06. was tested.

As a result, the methane conversion rate was 20.0%. The ethylene selectivity was 69.3% and the propylene selectivity was 1.1%. Furthermore, the selectivity for carbon monoxide was 8.7% and the selectivity for carbon dioxide was 10.8%. These values are all based on carbon.

Next, as Comparative Example 1, a test was performed in the same manner as in Example 1 except that the second gas did not contain water vapor and the molar ratio of oxygen per unit flow rate to methane was set to 0.08. .

As a result, the conversion of methane was 18.7%. The ethylene selectivity was 51.3% and the propylene selectivity was 1.0%. Furthermore, the selectivity for carbon monoxide was 8.8% and the selectivity for carbon dioxide was 29.4%. These values are all based on carbon.

Next, as Comparative Example 2, instead of introducing the first gas and the second gas into the catalyst layer through separate supply ports, a mixed gas of the first gas and the second gas (i.e., methane, steam and A test was conducted in the same manner as in Example 1 except that a mixed gas of oxygen) was introduced and the molar ratio of oxygen per unit flow rate to methane was set to 0.07. The configuration of Comparative Example 2 is the same as the configuration described in Patent Document 1 above, except that no hydrocarbon having 2 or more carbon atoms (such as ethane) is added after the OCM catalyst.

As a result, the conversion of methane was 18.6%. The ethylene selectivity was 55.4% and the propylene selectivity was 1.0%. Furthermore, the selectivity for carbon monoxide was 8.8% and the selectivity for carbon dioxide was 25.3%. These values are all based on carbon.

The above results are summarized in Table 1 below. In Table 1, the total olefin selectivity represents the sum of the ethylene selectivity and the propylene selectivity.

As shown in Examples 1 and 2, it was found that the selectivity of olefins (especially ethylene) can be increased by introducing the first gas and the second gas separately to the catalyst layer. In particular, it has been found that raising the reaction temperature suppresses the amount of carbon dioxide by-production and increases the selectivity of olefins (especially ethylene).

On the other hand, from the results of Comparative Examples 1 and 2, it was found that the olefin selectivity was still low although the use of steam slightly improved the olefin selectivity (Comparative Example 2). In particular, in Comparative Example 1 containing no steam, the carbon dioxide selectivity was high and the production amount increased. This is considered to be due to the fact that methane and oxygen are supplied to the catalyst layer 21 in a mixed state, so that methane is burned and carbon dioxide is increased (the selectivity of carbon dioxide is increased).

Thus, according to the reactor 100 described above, the selectivity of olefins (especially ethylene) can be increased. Also, the conversion rate of methane can be increased. This allows more methane to be converted to olefins, increasing the production of olefins. Furthermore, since the selectivity of carbon dioxide is kept low, carbon contained in the first gas such as natural gas or methane fermentation gas can be effectively used.

FIG. 3 is a cross-sectional view of a reactor 200 according to a second embodiment of the invention. In the reactor 200 , the first introduction part 26 made of, for example, a perforated plate has the same inner diameter as the catalyst container 25 . Between the introduction pipe 11 through which the first gas flows and the first introduction portion 26, a widening portion 34 is formed to widen the flow path. Therefore, the first gas is supplied to the entire upper surface of the catalyst layer 21 . Further, the spread portion 34 (first wall surface) is formed at a position facing the second wall surface 23 described above.

4 is a cross-sectional view taken along the line AA in FIG. 3. FIG. The first introduction portion 26 has a hole 26a. The holes 26 a are formed in a plurality of concentric circles at equal intervals in the circumferential direction of the circular first introduction portion 26 .

According to the reactor 200 , the first gas can be easily spread over the entire catalyst layer 21 . As a result, local reactions in the catalyst layer 21 can be suppressed, and reaction unevenness can be suppressed.

FIG. 5 is a cross-sectional view of a reactor 300 according to a third embodiment of the invention. The reactor 300 further includes a heating pipe 41 through which a heating gas flows, arranged so as to penetrate the catalyst layer 21 . The heating pipe 41 is arranged so as to vertically penetrate the catalyst layer 21 having a cylindrical shape. The heating gas flows upward inside the heating tube 41 .

The heating gas is, for example, flue gas or the like generated by combustion of fuel. Further, since the olefin produced in the catalyst layer 21 has heat, the heating gas may be the gas of the olefin discharged from the outlet 4 and having heat.

6 is a cross-sectional view taken along the line BB in FIG. 5. FIG. The heating tube 41 is flat. A plurality of heating pipes 41 are arranged at regular intervals in the circumferential direction of the cylindrical catalyst layer 21 . Thereby, the entire catalyst layer 21 can be heated by the heat of the heating gas flowing through the heating pipe 41 .

According to the reactor 300 described above, the catalyst layer 21 can be heated by the heating gas. Thereby, the production amount of olefin can be increased.

FIG. 7 is a cross-sectional view of a reactor 400 according to a fourth embodiment of the invention. In reactor 400, the first gas is fed in a direction similar to the direction of olefin withdrawal. Specifically, in the reactor 400 , both the first gas supply port 2 and the olefin discharge port 4 are arranged below the reactor 400 .

The catalyst container 25 includes a first wall surface 22 , a second wall surface 23 formed at a position facing the first wall surface 22 , and a side wall surface 24 connecting the first wall surface 22 and the second wall surface 23 . Of these, the first wall surface 22 is joined to the inner peripheral surface of the housing 1, and the first wall surface 22 divides the inner space of the housing 1 into an inner space 51 separate from the inner space 31 described above. be done.

The catalyst container 25 is a discharge channel for discharging the olefin produced in the catalyst layer 21, and extends between the first wall surface 22 and the second wall surface 23 and connects to the discharge part 27. The discharge channel forming member 53 is for example a pipe. The first introduction portion 26 and the discharge portion 27 are formed on the first wall surface 22 , and the second introduction portion is formed on the side wall surface 24 . Also, the second wall surface 23 forms the space 52 together with the upper surface 57 and the side wall surface 58 . The side wall surface 58 and the side wall surface 24 are formed integrally.

The olefin produced in the catalyst layer 21 is discharged to the space 52 through the sub-discharge part 29 (formed of, for example, a perforated plate) formed on the second wall surface 23 . The olefin discharged into the space 52 flows through the discharge channel forming member 53 and is discharged into the internal space. The olefin discharged into the internal space 51 is discharged outside the reactor 400 through the discharge port 4 .

According to the reactor 400, the heat of the olefin produced in the catalyst layer can be applied to the catalyst layer. Thereby, the catalyst layer can be heated.

1 Casing 2, 3 Supply port 4 Discharge port 11 Inlet pipe 12 Discharge pipe 21 Catalyst layer 22 First wall surface 23 Second wall surface 24, 58 Side wall surface 25 Catalyst container 26 First introduction part 26a Hole 27 Discharge part 28 Second introduction Part 29 Sub-discharge parts 31, 51 Internal space 32 First gas introduction channel 33 Second gas introduction channel 34 Spreading part 41 Heating tube 52 Space 53 Discharge channel forming member 57 Upper surface 100, 200, 300, 400 Reactor

Claims (11)

A reactor for producing olefins from a first gas containing methane using a partial oxidation coupling catalyst,
a housing;
a catalyst container disposed inside the housing, the catalyst container having therein a catalyst layer composed of the partial oxidation coupling catalyst;
a first gas introduction passage for introducing the first gas from the outside of the housing into the interior of the catalyst container through a first introduction portion formed in the catalyst container;
Vapor and oxygen are introduced into the catalyst container from the outside of the housing via a second introduction portion formed in the catalyst container and formed at a position different from the first introduction portion. a second gas introduction channel for introducing a second gas containing
with
The reactor, wherein the first gas and the second gas are separately introduced into the catalyst container . The catalyst container is formed with a discharge part for discharging the olefin produced in the catalyst layer,
2. The reactor according to claim 1, wherein the first introduction part is arranged so as to join the first gas with a gas flow from the second introduction part toward the discharge part. . one of the first gas introduction channel and the second gas introduction channel is formed by an internal space defined between the inner surface of the housing and the outer surface of the catalyst container;
The other of the first gas introduction channel and the second gas introduction channel is formed inside an introduction pipe extending in the internal space from the inner surface of the housing to the outer surface of the catalyst container. 3. Reactor according to claim 1 or 2, characterized in that it is the second gas introduction channel is formed by an internal space defined between the inner surface of the housing and the outer surface of the catalyst container;
3. The first gas introduction channel is formed inside an introduction pipe extending in the internal space from the inner surface of the housing to the outer surface of the catalyst container. The reactor described in . The catalyst container is formed with a discharge part for discharging the olefin produced in the catalyst layer,
The catalyst container includes a first wall surface, a second wall surface facing the first wall surface, and a side wall surface connecting the first wall surface and the second wall surface,
The first introduction portion is formed on the first wall surface,
The second introduction portion is formed on the side wall surface,
The reactor according to claim 3 or 4, wherein the discharge part is formed on the second wall surface. The catalyst container is formed with a discharge part for discharging the olefin produced in the catalyst layer,
The catalyst container is
a first wall surface;
a second wall surface formed at a position facing the first wall surface;
a side wall surface connecting the first wall surface and the second wall surface;
a discharge channel for discharging the olefin produced in the catalyst layer, the discharge channel extending between a first wall surface and a second wall surface and connecting to the discharge part; including a discharge channel forming member,
The first introduction portion and the discharge portion are formed on the first wall surface,
5. The reactor according to claim 3, wherein the second introduction part is formed on the side wall surface. The first gas introduction channel is
a first gas introduction main flow path for introducing the first gas from the outside of the housing into the interior of the catalyst container through a first main introduction portion formed on the first wall surface of the catalyst container;
a first gas introduction sub-flow path for introducing the first gas from the outside of the housing into the interior of the catalyst container through a first sub-introduction portion formed on the side wall surface of the catalyst container;
7. A reactor according to claim 5 or 6, characterized in that it comprises The reactor according to any one of claims 1 to 7, further comprising a heating pipe through which a heating gas flows, arranged so as to penetrate the catalyst layer. Reactor according to any one of claims 1 to 8, characterized in that the partial oxidation coupling catalyst comprises an alkali metal. the second gas includes methane;
The reaction according to any one of claims 1 to 9, wherein the second gas has a molar ratio of methane to oxygen contained in the second gas of 0.01 or more and 0.05 or less. vessel. A method for producing an olefin from a first gas containing methane using a partial oxidation coupling catalyst, comprising:
The first gas or the second gas containing water vapor and oxygen is supplied to a catalyst container arranged inside a housing, the catalyst container having a catalyst layer composed of the partial oxidation coupling catalyst inside. a first introduction step of introducing one of the gases;
a second introduction step of introducing the other of the first gas and the second gas into the catalyst container at a position different from the introduction part of the one gas;
including
A method for producing olefins, wherein the first gas and the second gas are separately introduced into the catalyst container .

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