CN115850001B - Method and device for preparing methane by combining carbon dioxide and hydrogen iodide - Google Patents
Method and device for preparing methane by combining carbon dioxide and hydrogen iodide Download PDFInfo
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Abstract
The invention discloses a method and a device for preparing methane by combining carbon dioxide with hydrogen iodide, which are characterized in that the hydrogen generated by hydrogen iodide decomposition reaction is consumed by introducing carbon dioxide hydrogenation to prepare methane, so that the decomposition of hydrogen iodide is promoted, meanwhile, the effect of promoting the decomposition hydrogen production is not achieved by increasing the reaction pressure on the hydrogen iodide decomposition reaction, but the reaction pressure has a positive promotion effect on the reaction of preparing methane by hydrogenating carbon dioxide, the hydrogen consumption is increased, the hydrogen generated by hydrogen iodide decomposition is consumed in situ, the hydrogen production process by hydrogen iodide decomposition is further promoted, namely, the hydrogen iodide decomposition rate is indirectly increased by more than 60% by increasing the pressure. After the hydrogen iodide decomposition reaction is combined with the methane preparation reaction by the carbon dioxide hydrogenation, hydrogen which is difficult to store and transport is directly converted into methane, and the methane can be transported by utilizing the existing natural gas pipeline, so that the problems of difficult storage and transportation of hydrogen energy are solved.
Description
Technical Field
The invention relates to the technical field of environmental protection and energy conservation, in particular to a method and a device for preparing methane by combining carbon dioxide and hydrogen iodide.
Background
Hydrogen energy is a well-known renewable clean energy source, and stands out in the great background of the era of low-carbon/zero-carbon energy sources. Among them, a hydrogen production method by thermochemical sulfur-iodine cycle (hereinafter referred to as sulfur-iodine cycle) has been attracting attention as one of the most ideal cycles in thermochemical hydrogen production methods. Sulfur iodine recycling has many unique advantages: (1) the reaction condition is relatively mild, and the heat sources such as solar energy, nuclear energy and the like can be matched; (2) the hydrogen production heat efficiency is high and can reach 60%; (3) the hydrogen and oxygen separation device is not needed, and the method is suitable for large-scale hydrogen production.
The sulfur-iodine circulation system mainly comprises a bunsen Bunshen reaction, sulfuric acid H 2 SO 4 Three schemes of decomposition and hydrogen iodide HI decomposition. The reaction principle of the three processes is as follows:
bunsen reaction: 2H (H) 2 O+SO 2 +I 2 →H 2 SO 4 +HI
H 2 SO 4 And (3) decomposition reaction: h 2 SO 4 →H 2 O+SO 2 +0.5O 2
HI decomposition reaction: HI→0.5H 2 +0.5I 2
Of the three schemes described above, HI catalytic decomposition is the most critical hydrogen production step. Because HI decomposition reaction is a reversible reaction, the hydrogen production efficiency by decomposition can only reach about 33% even at 700-800 ℃. How to increase the HI decomposition rate is a technical problem to be solved. In addition, due to the characteristics of small density, large volume, difficult compression and the like, the problem of high storage and transportation cost is encountered when the prepared hydrogen is stored. Suitable hydrogen storage technologies are therefore indispensable for the development of hydrogen energy sources today.
How to improve the hydrogen production efficiency by decomposing hydrogen iodide and reduce the energy consumption is a key problem. The hydrogen iodide decomposition hydrogen production reaction is a reversible reaction with lower hydrogen production efficiency, and HI is not basically decomposed at 400 ℃ under the condition of no catalyst; the HI decomposition rate at 500℃was also only 2%. Under the condition of using a catalyst, the HI decomposition rate is increased to 15-18% at 300 ℃, the HI decomposition rate is only increased to 20-22% at 500 ℃, the temperature is increased, the energy consumption for circularly heating HI gas is increased, but the decomposition rate is not increased well.
Disclosure of Invention
1. Technical problem to be solved by the invention
Aiming at the technical problems, the invention provides a method and a device for preparing methane by combining carbon dioxide with hydrogen iodide, which are used for introducing carbon dioxide to hydrogenate to prepare methane, consuming hydrogen generated by hydrogen iodide decomposition reaction, promoting the decomposition of hydrogen iodide and solving the problem of hydrogen energy storage and transportation.
2. Technical proposal
In order to solve the problems, the technical scheme provided by the invention is as follows: a method for preparing methane by combining carbon dioxide and hydrogen iodide, comprising the following steps:
(1) Delivering hydrogen iodide gas to a hydrogen iodide pre-decomposer, and carrying out catalytic decomposition to generate mixed gas A, wherein the mixed gas comprises hydrogen iodide, iodine vapor and hydrogen;
(2) Fully mixing carbon dioxide and the mixed gas A in a gas premixer to obtain mixed gas B, wherein the temperature of the mixed gas B is controlled at 300-400 ℃;
(3) Delivering the mixed gas B to a methane synthesizer, wherein the reaction temperature is 300-400 ℃, the reaction pressure is 5-15 MPa, and the mixed gas C is obtained through catalytic reaction, and comprises methane, carbon dioxide, water vapor, hydrogen iodide, iodine vapor and hydrogen;
(4) And (3) the mixed gas C enters a cooling separator, the temperature is cooled to 85-105 ℃, iodine solid, liquid water and mixed gas D are separated, the mixed gas D comprises methane, carbon dioxide, hydrogen iodide and hydrogen, and methane is obtained by separation of the methane separator.
Optionally, the mixed gas D in the step (4) is separated into methane and mixed gas E by a methane separator, the mixed gas E is conveyed to a carbon dioxide separator to separate carbon dioxide gas, the carbon dioxide gas is conveyed to a gas pre-mixer for recycling, and the rest hydrogen iodide gas and hydrogen gas are conveyed to a hydrogen iodide pre-decomposer for recycling.
Optionally, the reaction temperature in the step (1) is 300-500 ℃.
Optionally, in the step (2), the molar ratio of carbon dioxide to hydrogen iodide is 1:6 to 8.
Optionally, the catalysts in the step (1) and the step (3) are nickel metal particle supported catalysts.
Optionally, the carrier of the nickel metal particles loaded in the catalyst is silicon dioxide, aluminum oxide, titanium dioxide, magnesium oxide, cerium dioxide, zinc dioxide or activated carbon.
The invention also discloses a device for preparing methane by combining carbon dioxide with hydrogen iodide, which comprises a hydrogen iodide pre-decomposer, a gas pre-mixer, a methane synthesizer, a cooling separator, a methane separator and a carbon dioxide separator which are sequentially connected, wherein the hydrogen iodide pre-decomposer is connected with a hydrogen iodide gas tank, the gas pre-mixer is connected with a carbon dioxide gas tank, the methane separator is connected with a methane gas tank, and the carbon dioxide separator is connected with the gas pre-mixer, wherein: the hydrogen iodide tank is used for storing hydrogen iodide gas; the carbon dioxide gas tank is used for storing carbon dioxide gas; the hydrogen iodide pre-decomposer is used for decomposing hydrogen iodide; the gas premixer is used for mixing carbon dioxide and gas from the hydrogen iodide pre-decomposer; the methane synthesizer is used for synthesizing methane; the cooling separator is used for separating iodine solid and water; the methane separator is used for separating methane; the carbon dioxide separator is used for separating carbon dioxide, the separated carbon dioxide is conveyed to the gas pre-mixer for recycling, and the rest hydrogen iodide gas and hydrogen gas are conveyed to the hydrogen iodide pre-decomposer for recycling.
Optionally, the methane synthesizer is a tubular fixed bed reactor, and a catalyst is filled in a reaction tube of the tubular fixed bed reactor.
3. Advantageous effects
Compared with the prior art, the technical scheme provided by the invention has the following beneficial effects:
(1) According to the method for preparing methane by combining carbon dioxide with hydrogen iodide, the reaction of preparing methane by introducing carbon dioxide hydrogenation consumes hydrogen generated by hydrogen iodide decomposition reaction, so that the decomposition of hydrogen iodide is promoted, meanwhile, as the effect of promoting the decomposition hydrogen production on the hydrogen iodide decomposition reaction is not achieved by increasing the reaction pressure, the forward promotion reaction of the reaction of preparing methane by hydrogenating carbon dioxide by the reaction pressure is achieved, the hydrogen consumption is increased, the hydrogen generated by hydrogen iodide decomposition is consumed in situ, and the hydrogen production process by hydrogen iodide decomposition is further promoted. Namely, the pressure is increased to indirectly increase the decomposition rate of the hydrogen iodide by more than 60 percent.
(2) According to the method for preparing methane by combining carbon dioxide with hydrogen iodide, which is provided by the embodiment of the application, after the hydrogen iodide decomposition reaction is combined with the reaction for preparing methane by hydrogenating carbon dioxide, hydrogen which is difficult to store and transport is directly converted into methane. And methane can be transported by using the existing natural gas pipeline, so that the problem of difficult storage and transportation of hydrogen energy is solved.
(3) According to the method for preparing methane by combining carbon dioxide with hydrogen iodide, which is provided by the embodiment of the application, the methane is synthesized by the carbon dioxide and the hydrogen, so that the effect of recycling the carbon dioxide is realized.
Drawings
FIG. 1 is a schematic flow chart of a method for preparing methane by combining carbon dioxide with hydrogen iodide according to an embodiment of the invention.
Detailed Description
For a further understanding of the present invention, the present invention will be described in detail with reference to the drawings and examples.
The present application is described in further detail below with reference to the drawings and examples. It is to be understood that the specific embodiments described herein are merely illustrative of the invention and are not limiting of the invention. It should be noted that, for convenience of description, only the portions related to the invention are shown in the drawings. The first, second, etc. words are provided for convenience in describing the technical scheme of the present invention, and have no specific limitation, and are all generic terms, and do not constitute limitation to the technical scheme of the present invention. It should be noted that, in the case of no conflict, the embodiments and features in the embodiments may be combined with each other. In the description of the present invention, it should be noted that the directions or positional relationships indicated by the terms "center", "upper", "lower", "left", "right", "vertical", "horizontal", "inner", "outer", etc. are based on the directions or positional relationships shown in the drawings, are merely for convenience of describing the present invention and simplifying the description, and do not indicate or imply that the devices or elements referred to must have a specific orientation, be configured and operated in a specific orientation, and thus should not be construed as limiting the present invention. Furthermore, the terms "first," "second," and "third" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance. Unless specifically stated or limited otherwise, the terms "mounted," "connected," and "coupled" are to be construed broadly, and may be, for example, fixedly connected, detachably connected, or integrally connected; can be mechanically or electrically connected; can be directly connected or indirectly connected through an intermediate medium, and can be communication between two elements. The specific meaning of the above terms in the present invention will be understood in specific cases by those of ordinary skill in the art. The technical schemes in the same embodiment and the technical schemes in different embodiments can be arranged and combined to form a new technical scheme without contradiction or conflict, which is within the scope of the invention.
Description of principle:
in this example, hydrogen and carbon dioxide are used as raw materials to react to prepare methane. Carbon dioxide and hydrogen are adsorbed on the surface of the catalyst loaded with metal particles and gradually converted into gaseous methane CH 4 . Methane can be transported by using the existing natural gas pipeline, and is hydrogen for a long distance>200 km) and solves the problem of difficult storage and transportation of hydrogen energy. The reaction temperature is controlled between 300 and 500 ℃ and the reaction pressure is controlled between 5 and 15MPa in the system. The reaction formula is as follows:
this example requires pressurizing the reactor. When the temperature in the reaction vessel is controlled between 300 and 500 ℃, HI and H are controlled 2 O、I 2 、CO、CO 2 、H 2 CH (CH) 4 Are all in a gaseous state. At this time, the effect of the total reaction pressure on the reaction involving the gas is as follows:
assuming that the reaction isWherein the four of the ABCD are gases,
when the total number of the reactant and the resultant gas molecules is the same, namely a+b=c+d, increasing the total reaction pressure does not affect the chemical equilibrium, namely the chemical equilibrium does not shift;
when the total number of the reactant and the resultant molecules is different, i.e., a+b+.c+d, the total pressure of the reaction is increased, and the chemical equilibrium is shifted in the direction of decreasing the total number of the gas molecules. The total reaction pressure is reduced, and the chemical equilibrium is shifted in the direction of increasing the total number of gas molecules.
Comparing the hydrogen iodide decomposition reaction and the methane production reaction by the hydrogenation of carbon dioxide, it can be found that: (1) The total number of the reactant and the gas molecules of the product is the same, so that the change of the total pressure of the reaction has no influence on the chemical balance, namely the total pressure is increased, and the decomposition of the hydrogen iodide cannot be promoted; (2) In the reaction of preparing methane by hydrogenating carbon dioxide, the total number of molecules of reactants is larger than that of the products, so that if the total pressure of the reaction is increased, the chemical equilibrium moves to the direction of generating the products, namely more carbon dioxide and hydrogen are consumed, and more methane is generated; (3) In the present system, increasing the total pressure of the reaction promotes shifting of the chemical equilibrium of the two reactions in the direction of the production of the product. Because the hydrogen consumed by the reaction for preparing methane by hydrogenating carbon dioxide comes from the hydrogen iodide decomposition reaction, the total reaction pressure is increased, the hydrogen consumption in the reaction for preparing methane by hydrogenating carbon dioxide is promoted, and the hydrogen consumption promotes the chemical balance of the hydrogen iodide decomposition reaction to move towards the hydrogen production direction, namely the hydrogen production by decomposing hydrogen iodide is promoted.
As shown in fig. 1, the invention provides a method for preparing methane by combining carbon dioxide and hydrogen iodide, which comprises the following steps:
(1) Delivering hydrogen iodide gas to a hydrogen iodide pre-decomposer, and carrying out catalytic decomposition at the temperature of 300-500 ℃ to generate mixed gas A, wherein the mixed gas comprises hydrogen iodide, iodine vapor and hydrogen; part of the hydrogen iodide gas comes from a sulfur iodine circulating system, and the other part comes from a carbon dioxide separator, and carbon dioxide CO 2 A part of the gas is supplied from the outside,the other part comes from the carbon dioxide separator, HI gas is pre-decomposed in the hydrogen iodide pre-decomposer, and part of hydrogen is generated to accelerate and improve the methane synthesis efficiency. The catalyst is a nickel-based catalyst (preferably a Ni/AC catalyst). In the hydrogen iodide pre-decomposer, about 15% to 20% of HI gas is decomposed, and mixed gas A includes hydrogen iodide, iodine vapor and hydrogen.
(2) Fully mixing carbon dioxide and the mixed gas A in a gas premixer to obtain mixed gas B, wherein the temperature of the mixed gas B is controlled at 300-400 ℃; because the catalyst is filled in the methane synthesizer in the subsequent step, if the two gases are directly introduced, the mixing of the gases between the gaps of the catalyst requires time and space, thus increasing the volume of the methane synthesizer and reducing the efficiency of methane synthesis. In addition, the temperature of the mixed gas in the gas premixer needs to be adjusted. Research shows that the high temperature (300-500 ℃) has an inhibiting effect on the reaction of preparing methane by hydrogenating carbon dioxide, but has a promoting effect on the hydrogen production reaction by decomposing hydrogen iodide, and the reaction temperature of entering a methane synthesizer needs to be controlled at 300-400 ℃ in order to balance the two. Therefore, the mixing temperature in the gas premixer is controlled by using low-temperature carbon dioxide gas, and the molar ratio of the carbon dioxide to the hydrogen iodide in the mixed gas is 1:6 to 8.
(3) Delivering the mixed gas B to a methane synthesizer, wherein the reaction temperature is 300-400 ℃, the reaction pressure is 5-15 MPa, and the mixed gas C is obtained under the catalysis of a catalyst, and comprises methane, carbon dioxide, water vapor, hydrogen iodide, iodine vapor and hydrogen; the methane synthesis reactor uses a tubular fixed bed reactor, a granular catalyst, namely a catalyst loaded with Ni metal particles, is filled in a reaction tube, and the carrier loaded with the metal particles is: siO (SiO) 2 、Al 2 O 3 、TiO 2 、MgO、CeO 2 、ZrO 2 And an AC.
(4) And (3) the mixed gas C enters a cooling separator, the temperature is cooled to 85-105 ℃, at the moment, iodine vapor and water vapor are separated out, the iodine simple substance is solid, and the water is liquid. Separating iodine solid, liquid water and mixed gas D, separating the iodine solid from the water, and then allowing the residual mixed gas D to enter a methane separator to separate methane gas and mixed gas E. The mixed gas D includes methane, carbon dioxide, hydrogen iodide, and hydrogen.
(5) And the mixed gas E is conveyed to a carbon dioxide separator to separate carbon dioxide gas, the carbon dioxide gas is conveyed to a gas pre-mixer for recycling, and the rest hydrogen iodide gas and hydrogen gas are conveyed to a hydrogen iodide pre-decomposer for recycling, so that the hydrogen which is difficult to store and transport is conveniently and directly converted into methane, and the methane can be transported by utilizing the existing natural gas pipeline, thereby solving the problems of difficult storage and transportation of hydrogen energy.
The invention also provides a device for preparing methane by combining carbon dioxide with hydrogen iodide, which comprises a hydrogen iodide pre-decomposer, a gas pre-mixer, a methane synthesizer, a cooling separator, a methane separator and a carbon dioxide separator which are sequentially connected, wherein the hydrogen iodide pre-decomposer is connected with a hydrogen iodide gas tank, the gas pre-mixer is connected with a carbon dioxide gas tank, the methane separator is connected with a methane gas tank, and the carbon dioxide separator is connected with the gas pre-mixer, wherein: the hydrogen iodide tank is used for storing hydrogen iodide gas; the carbon dioxide gas tank is used for storing carbon dioxide gas; the hydrogen iodide pre-decomposer is used for decomposing hydrogen iodide; the gas premixer is used for mixing carbon dioxide and gas from the hydrogen iodide pre-decomposer; the methane synthesizer is used for synthesizing methane; the cooling separator is used for separating iodine solid and water; the methane separator is used for separating methane; the carbon dioxide separator is used for separating carbon dioxide, the separated carbon dioxide is conveyed to the gas pre-mixer for recycling, and the rest hydrogen iodide gas and hydrogen gas are conveyed to the hydrogen iodide pre-decomposer for recycling.
The method introduces the reaction of preparing methane by carbon dioxide hydrogenation, consumes hydrogen generated by the hydrogen iodide decomposition reaction, and promotes the decomposition of hydrogen iodide. Meanwhile, the effect of the reaction pressure on hydrogen iodide decomposition reaction does not promote the decomposition hydrogen production, but the reaction pressure positively promotes the reaction of the reaction for preparing methane by hydrogenating carbon dioxide, so that the hydrogen consumption is increased, the hydrogen produced by hydrogen iodide decomposition is consumed in situ, and the hydrogen production process by hydrogen iodide decomposition is further promoted. Namely, the pressure is increased to indirectly increase the decomposition rate of the hydrogen iodide by more than 60 percent.
Example 1
(1) After the device for preparing methane by combining carbon dioxide and hydrogen iodide stably operates, HI gas is introduced into a hydrogen iodide pre-decomposer, wherein one part of HI gas flows into the hydrogen iodide pre-decomposer from a hydrogen iodide gas tank at 48kg/h, the other part of HI gas flows into the hydrogen iodide pre-decomposer from a carbon dioxide separator at 202kg/h, the gas is heated to about 500 ℃ in the hydrogen iodide pre-decomposer, a reaction chamber of the hydrogen iodide pre-decomposer is filled with a loaded activated carbon catalyst, and about 18% of HI gas is decomposed into iodine simple substance and hydrogen under the catalytic action of the catalyst to form mixed gas A.
(2) The mixed gas A enters a gas premixer and CO 2 The gas enters a gas pre-mixer, wherein a part of CO 2 The gas enters a gas pre-mixer from a carbon dioxide gas tank at a flow rate of 4.29kg/h, and the other part of CO 2 The gas from the carbon dioxide separator was fed into the gas pre-mixer at a flow rate of 6.45kg/h, where the three gases were thoroughly mixed and heated to 350 c to form a mixed gas B.
(3) The mixed gas B enters a methane synthesizer, the reaction temperature is 350 ℃, the reaction pressure is controlled to be 10MPa, and the catalyst is Ni/SiO 2 And (3) reacting the mixed gas B to generate methane and water to form mixed gas C.
(4) The mixed gas C enters a cooling separator, the temperature is reduced to 87 ℃, and iodine vapor and water vapor are changed into iodine solid and liquid water to be separated. The mixed gas then enters a methane separator, methane is separated, and the yield of methane is 1.17kg/h. The HI gas comprehensive decomposition hydrogen production rate in the system reaches 42.56%, and is improved by 136.4% compared with the decomposition hydrogen production rate of a hydrogen iodide pre-decomposer. The mixed gas after methane separation is mixed gas E, and the mixed gas E comprises carbon dioxide, hydrogen iodide and hydrogen.
(5) And the mixed gas E is conveyed to a carbon dioxide separator to separate carbon dioxide gas, the carbon dioxide gas is conveyed to a gas pre-mixer for recycling, and the rest hydrogen iodide gas and hydrogen gas are conveyed to a hydrogen iodide pre-decomposer for recycling, so that the hydrogen which is difficult to store and transport is conveniently and directly converted into methane, and the methane can be transported by utilizing the existing natural gas pipeline, thereby solving the problems of difficult storage and transportation of hydrogen energy.
Example 2
(1) After the device for preparing methane by combining carbon dioxide and hydrogen iodide stably operates, HI gas is introduced into a hydrogen iodide pre-decomposer, wherein one part of HI gas flows into the hydrogen iodide pre-decomposer from a hydrogen iodide gas tank at 98.4kg/h, the other part of HI gas flows into the hydrogen iodide pre-decomposer from a carbon dioxide separator at 401.6kg/h, the gas is heated to about 500 ℃ in the hydrogen iodide pre-decomposer, a reaction chamber of the hydrogen iodide pre-decomposer is filled with a loaded activated carbon catalyst, and about 15% of HI gas is decomposed into iodine simple substance and hydrogen under the catalytic action of the catalyst to form mixed gas A.
(2) The mixed gas A enters a gas premixer and CO 2 The gas enters a gas premixer, a part of CO 2 The gas enters a gas pre-mixer from a carbon dioxide gas tank at a flow rate of 6.62kg/h, and the other part of CO 2 The gas from the carbon dioxide separator was fed into the gas pre-mixer at a flow rate of 22.18 kg/h. The three gases were thoroughly mixed in a gas premixer and heated to 320 ℃ to form a mixed gas B.
(3) The mixed gas B enters a methane synthesizer, the reaction temperature is 320 ℃, the reaction pressure is controlled to be 15MPa, and the catalyst is Ni/SiO 2 AC. And (3) generating methane and water after the mixed gas B reacts to form mixed gas C.
(4) The mixed gas C enters a first-stage cooling separator, the temperature is reduced to 85 ℃, and iodine vapor and water vapor are changed into iodine solid and liquid water to be separated. The mixed gas then enters a methane separator, methane is separated, and the yield of methane is 2.05kg/h. The HI gas comprehensive decomposition hydrogen production rate in the system reaches 29.80 percent, and compared with the decomposition hydrogen production rate of a hydrogen iodide pre-decomposer, the HI gas comprehensive decomposition hydrogen production rate is improved by 98.6 percent. The mixed gas after methane separation is mixed gas E, and the mixed gas E comprises carbon dioxide, hydrogen iodide and hydrogen.
(5) And the mixed gas E is conveyed to a carbon dioxide separator to separate carbon dioxide gas, the carbon dioxide gas is conveyed to a gas pre-mixer for recycling, and the rest hydrogen iodide gas and hydrogen gas are conveyed to a hydrogen iodide pre-decomposer for recycling, so that the hydrogen which is difficult to store and transport is conveniently and directly converted into methane, and the methane can be transported by utilizing the existing natural gas pipeline, thereby solving the problems of difficult storage and transportation of hydrogen energy.
The invention and its embodiments have been described above by way of illustration and not limitation, and the invention is illustrated in the accompanying drawings and described in the drawings in which the actual structure is not limited thereto. Therefore, if one of ordinary skill in the art is informed by this disclosure, the structural mode and the embodiments similar to the technical scheme are not creatively designed without departing from the gist of the present invention.
Claims (8)
1. A method for preparing methane by combining carbon dioxide and hydrogen iodide, which is characterized by comprising the following steps:
(1) Delivering hydrogen iodide gas to a hydrogen iodide pre-decomposer, and carrying out catalytic decomposition to generate mixed gas A, wherein the mixed gas comprises hydrogen iodide, iodine vapor and hydrogen;
(2) Fully mixing carbon dioxide and the mixed gas A in a gas premixer to obtain mixed gas B, wherein the temperature of the mixed gas B is controlled at 300-400 ℃;
(3) Delivering the mixed gas B to a methane synthesizer, wherein the reaction temperature is 300-400 ℃, the reaction pressure is 5-15 MPa, and the mixed gas C is obtained through catalytic reaction, and comprises methane, carbon dioxide, water vapor, hydrogen iodide, iodine vapor and hydrogen;
(4) And (3) the mixed gas C enters a cooling separator, the temperature is cooled to 85-105 ℃, iodine solid, liquid water and mixed gas D are separated, the mixed gas D comprises methane, carbon dioxide, hydrogen iodide and hydrogen, and methane is obtained by separation of the methane separator.
2. The method for preparing methane by combining carbon dioxide with hydrogen iodide according to claim 1, wherein the mixed gas D in the step (4) is separated into methane and mixed gas E by a methane separator, the mixed gas E is conveyed to a carbon dioxide separator, the carbon dioxide gas is separated, the carbon dioxide gas is conveyed to a gas pre-mixer for recycling, and the rest of the hydrogen iodide gas and hydrogen gas are conveyed to a hydrogen iodide pre-decomposer for recycling.
3. The method for producing methane by combining carbon dioxide with hydrogen iodide according to claim 1, wherein the reaction temperature in the step (1) is 300 to 500 ℃.
4. The method for producing methane by combining carbon dioxide with hydrogen iodide according to claim 1, wherein the molar ratio of carbon dioxide to hydrogen iodide in the step (2) is 1:6 to 8.
5. The method for producing methane by combining carbon dioxide with hydrogen iodide according to claim 1, wherein the catalysts in the step (1) and the step (3) are nickel metal particle-supported catalysts.
6. The method for preparing methane by combining carbon dioxide with hydrogen iodide according to claim 5, wherein the carrier loading nickel metal particles in the catalyst is silica, aluminum oxide, titanium dioxide, magnesium oxide, cerium oxide, zinc oxide or activated carbon.
7. The utility model provides a device of hydrogen iodide preparation methane is united to carbon dioxide, its characterized in that, including hydrogen iodide predecomposition ware, gas premixer, methane synthesizer, cooling separator, methane separator and the carbon dioxide separator that connects gradually, hydrogen iodide predecomposition ware is connected with the hydrogen iodide gas pitcher, gas premixer is connected with the carbon dioxide gas pitcher, methane separator is connected with the methane gas pitcher, the carbon dioxide separator is connected with gas premixer, wherein:
the hydrogen iodide tank is used for storing hydrogen iodide gas;
the carbon dioxide gas tank is used for storing carbon dioxide gas;
the hydrogen iodide pre-decomposer is used for decomposing hydrogen iodide;
the gas premixer is used for mixing carbon dioxide and gas from the hydrogen iodide pre-decomposer;
the methane synthesizer is used for synthesizing methane;
the cooling separator is used for separating iodine solid and water;
the methane separator is used for separating methane;
the carbon dioxide separator is used for separating carbon dioxide, the separated carbon dioxide is conveyed to the gas pre-mixer for recycling, and the rest hydrogen iodide gas and hydrogen gas are conveyed to the hydrogen iodide pre-decomposer for recycling.
8. The apparatus for producing methane by combining carbon dioxide with hydrogen iodide according to claim 7, wherein the methane synthesizer is a tubular fixed bed reactor, and a reaction tube of the tubular fixed bed reactor is filled with a catalyst.
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