CN117427570A - Methane preparation system and methane preparation method - Google Patents
Methane preparation system and methane preparation method Download PDFInfo
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- CN117427570A CN117427570A CN202311322028.2A CN202311322028A CN117427570A CN 117427570 A CN117427570 A CN 117427570A CN 202311322028 A CN202311322028 A CN 202311322028A CN 117427570 A CN117427570 A CN 117427570A
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 title claims abstract description 242
- 238000002360 preparation method Methods 0.000 title abstract description 21
- 238000003786 synthesis reaction Methods 0.000 claims abstract description 312
- 230000015572 biosynthetic process Effects 0.000 claims abstract description 284
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 62
- 239000007788 liquid Substances 0.000 claims abstract description 42
- 238000001816 cooling Methods 0.000 claims abstract description 34
- 238000000926 separation method Methods 0.000 claims abstract description 30
- 238000004519 manufacturing process Methods 0.000 claims abstract description 19
- 230000009467 reduction Effects 0.000 claims abstract description 8
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical class [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 33
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 27
- 238000006243 chemical reaction Methods 0.000 claims description 27
- 239000003054 catalyst Substances 0.000 claims description 26
- 230000001105 regulatory effect Effects 0.000 claims description 21
- 230000002194 synthesizing effect Effects 0.000 claims description 21
- 238000010438 heat treatment Methods 0.000 claims description 17
- 229910002090 carbon oxide Inorganic materials 0.000 claims description 14
- 238000000034 method Methods 0.000 claims description 12
- 238000006555 catalytic reaction Methods 0.000 claims description 10
- 229910052759 nickel Inorganic materials 0.000 claims description 9
- 238000004891 communication Methods 0.000 claims description 3
- 239000007789 gas Substances 0.000 description 188
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 24
- 229910002091 carbon monoxide Inorganic materials 0.000 description 19
- 229910002092 carbon dioxide Inorganic materials 0.000 description 12
- 239000001569 carbon dioxide Substances 0.000 description 12
- 239000000047 product Substances 0.000 description 8
- 238000005265 energy consumption Methods 0.000 description 7
- 239000001257 hydrogen Substances 0.000 description 7
- 229910052739 hydrogen Inorganic materials 0.000 description 7
- 230000008569 process Effects 0.000 description 5
- 238000011084 recovery Methods 0.000 description 5
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 4
- 238000013461 design Methods 0.000 description 4
- 239000002994 raw material Substances 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 230000001276 controlling effect Effects 0.000 description 3
- 238000005315 distribution function Methods 0.000 description 3
- 150000002431 hydrogen Chemical class 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 230000006835 compression Effects 0.000 description 2
- 238000007906 compression Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000011068 loading method Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000000746 purification Methods 0.000 description 2
- 230000036632 reaction speed Effects 0.000 description 2
- 239000002028 Biomass Substances 0.000 description 1
- OBOXTJCIIVUZEN-UHFFFAOYSA-N [C].[O] Chemical class [C].[O] OBOXTJCIIVUZEN-UHFFFAOYSA-N 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000002309 gasification Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000012946 outsourcing Methods 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 238000009423 ventilation Methods 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
- C07C1/02—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
- C07C1/04—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon monoxide with hydrogen
- C07C1/0405—Apparatus
- C07C1/041—Reactors
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
- B01J8/0242—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid flow within the bed being predominantly vertical
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
- B01J8/0285—Heating or cooling the reactor
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
- C07C1/02—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
- C07C1/12—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon dioxide with hydrogen
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
- C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
- C10L3/08—Production of synthetic natural gas
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C2523/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00
- C07C2523/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00 of the iron group metals or copper
- C07C2523/74—Iron group metals
- C07C2523/755—Nickel
Abstract
The invention provides a methane preparation system and a methane preparation method. The methane production system comprises: a first heat exchange device comprising a first heat channel and a first medium channel; the first synthesis equipment is used for carrying out methane synthesis reaction to obtain first tower post-gas; the second synthesis equipment is used for receiving the synthesis gas after temperature rise and the first post-tower gas after temperature reduction; a second heat exchange device comprising a second heat channel and a second media channel; the gas-liquid separation equipment is used for receiving the cooled second tower post gas and performing gas-liquid separation to separate out water; the pressurizing device is arranged at the downstream of the gas-liquid separation device and is used for receiving the second post-tower gas after water separation and pressurizing to obtain circulating gas; a third synthesis device to receive the recycle gas and to provide the recycle gas for methane synthesis reaction; and the cooling and separating equipment is used for receiving the synthesized primary methane, cooling the primary methane and separating gas from liquid to obtain a methane product.
Description
Technical Field
The invention relates to the technical field of methane preparation, in particular to a methane preparation system and a methane preparation method.
Background
The current methane synthesis process mainly comprises an adiabatic methanation methane synthesis process with circulation and an isothermal methanation methane synthesis process without circulation.
In the isothermal methanation process for synthesizing methane, the methanation reaction speed is high, the temperature of a reaction hot spot is close to the equilibrium temperature, and the temperature of the methanation hot spot is very high for raw material gas with higher carbon monoxide and carbon dioxide content, so that carbon precipitation reaction is easy to occur at the moment to cause the methanation catalyst to lose efficacy. Although the control of the methanation hotspot temperature can be achieved by directly adding a large amount of steam to the feed gas to dilute the carbon monoxide and carbon dioxide concentrations in the feed gas, the energy consumption is extremely high due to the need to directly add a large amount of steam. For raw material gas with lower carbon monoxide and carbon dioxide content, the isothermal reaction removes heat, so that the temperature of a methanation hot spot is not high, the methanation reaction speed is reduced along with the temperature reduction, and the catalyst efficiency is reduced.
In the adiabatic methanation process for synthesizing methane, the reacted methane gas is returned to dilute the concentration of carbon monoxide and carbon dioxide in the raw material gas to control the temperature of methanation hot spots, and the equilibrium concentration of carbon monoxide and carbon dioxide in the reacted gas is higher due to higher temperature after adiabatic reaction. For the raw material gas with higher carbon monoxide and carbon dioxide content, in order to control the temperature of methanation hot spots, the circulation amount needs to be increased, the number of adiabatic methanation reactors is increased, and meanwhile, related facilities for recovering the high-temperature heat of the adiabatic methanation reaction gas are also increased, so that the investment is larger, and the energy consumption is relatively higher.
Disclosure of Invention
The invention aims to provide a methane preparation system with low energy consumption and a methane preparation method, so as to solve the problems in the prior art.
In order to solve the above technical problems, the present invention provides a methane preparation system, comprising:
a first heat exchange device including a first heat channel and a first medium channel which are independent of each other and capable of heat exchange; the inlet of the first medium channel is used for receiving outside synthesis gas, and the inlet of the first medium channel is used for receiving outside synthesis gas (H 2 -CO 2 )/(CO+CO 2 ) Is greater than 3 volume percent;
the first synthesis equipment is connected with the outlet of the first medium channel so as to receive the warmed synthesis gas; the first synthesis equipment is used for carrying out methane synthesis reaction to obtain first tower post gas; the outlet of the first synthesis device communicates with the inlet of the first heat channel to provide the first column off-gas;
the inlet of the second synthesis equipment is connected with the outlet of the first medium channel and the outlet of the first heat channel at the same time and is used for receiving the synthesis gas after temperature rise and the first tower post gas after temperature reduction; the second synthesis equipment is used for carrying out methane synthesis reaction to obtain second tower post gas;
a second heat exchange device including a second heat channel and a second medium channel which are independent of each other and capable of heat exchange; the inlet of the second heat channel is connected with the second synthesis equipment to receive the second post-tower gas; the outlet of the second medium channel is communicated with the inlet of the first synthesis equipment;
the gas-liquid separation device is arranged at the downstream of the second heat channel and used for receiving the cooled second tower post gas and performing gas-liquid separation to separate water;
the pressurizing device is arranged at the downstream of the gas-liquid separation device and is used for receiving the second tower post gas after water is separated and pressurizing to obtain circulating gas, and the pressurizing device is communicated with the inlet of the second medium channel;
a third synthesis device disposed in parallel with the first synthesis device and downstream of the second media path to receive the recycle gas and provide the recycle gas for methane synthesis reactions;
the cooling and separating device is arranged at the downstream of the third synthesizing device to receive the synthesized primary methane and cool the primary methane and separate gas from liquid to obtain a methane product.
In one embodiment, a first flow regulating valve is arranged between the first medium channel and the first synthesizing device; and/or the number of the groups of groups,
and a second flow regulating valve is arranged between the first medium channel and the second synthesizing equipment.
In one embodiment, a steam superheater is further arranged between the first synthesis device and the first heat channel, the steam superheater comprises a heating pipeline, steam is used for passing through the heating pipeline, the steam absorbs heat of the first tower back gas to form superheated steam, and an outlet of the heating pipeline is communicated with an inlet of the second synthesis device to input the superheated steam to the second synthesis device.
In one embodiment, a first steam generator is further arranged between the second synthesis device and the second heat exchange device, the first steam generator comprises a first water supply pipeline for water supply circulation, the second post-tower gas is used for providing heat for water in the first water supply pipeline so as to enable the water to be converted into steam, and an outlet of the first water supply pipeline is communicated with a heating pipeline of the steam superheater.
In one embodiment, a first cooling device is further arranged between the second heat exchange device and the gas-liquid separation device.
In one embodiment, the cooling and separating device comprises a second steam generator and a gas-liquid separator;
the second steam generator comprises a second water supply pipeline for water supply circulation, the primary methane is used for providing heat for water in the second water supply pipeline so as to enable the water to be converted into steam, and the gas-liquid separator is used for receiving the primary methane after temperature reduction and performing gas-liquid separation to obtain methane products.
In one embodiment, a second cooling device is further arranged between the second steam generator and the gas-liquid separator.
In one embodiment, the first synthesis apparatus is packed with a nickel catalyst, the second synthesis apparatus is packed with a nickel catalyst, and the third synthesis apparatus is packed with a nickel catalyst.
In one embodiment, the first synthesis apparatus, the second synthesis apparatus, and the third synthesis apparatus are all shaft radial adiabatic synthesis reactors.
The invention also provides a preparation method of methane, which comprises the following steps:
providing synthesis gas, wherein (H) 2 -CO 2 )/(CO+CO 2 ) Is greater than 3 volume percent;
the synthesis gas is heated by heat exchange and then enters into first synthesis equipment and second synthesis equipment respectively;
methane synthesis reaction is carried out in the first synthesis equipment to obtain first tower post gas;
the first post-tower gas and the synthesis gas enter the second synthesis equipment after heat exchange and temperature reduction, and the first post-tower gas and the synthesis gas jointly perform methane synthesis reaction in the second synthesis equipment to obtain second post-tower gas;
cooling the second tower post gas, and then performing gas-liquid separation to separate water from the second tower post gas;
pressurizing the second tower gas after water separation to form circulating gas, carrying out heat exchange and heating on the circulating gas and the second tower gas, and then entering the first synthesis equipment and the third synthesis equipment, and carrying out methane synthesis reaction in the third synthesis equipment to obtain primary methane;
and cooling and gas-liquid separating the primary methane to obtain the product methane.
In one embodiment, the method further comprises the following steps:
adjusting the amount of the synthesis gas entering the first synthesis equipment to make the mole percentage of the total carbon oxides in the synthesis gas and the recycle gas in the first synthesis equipment be 3.0-5.0%; and/or the number of the groups of groups,
the amount of the synthesis gas entering the second synthesis equipment is regulated so that the mole percentage of the total carbon oxides in the synthesis gas and the second post-tower gas in the second synthesis equipment is 3.0-10.0%.
In one embodiment, before the heat exchange between the second post-tower gas and the recycle gas, the method further comprises the following steps:
and the second post-tower gas exchanges heat with water, releases heat to convert the water into steam, exchanges heat with the circulating gas after cooling, and exchanges heat with the first post-tower gas.
In one embodiment, before the heat exchange between the first post-tower gas and the synthesis gas, the method further comprises the following steps:
and the first post-tower gas exchanges heat with the steam, releases heat to convert the steam into superheated steam, and the superheated steam enters the second synthesis equipment, and exchanges heat with the synthesis gas.
In one embodiment, the synthesis gas and the recycle gas enter from the top of the first synthesis equipment and pass through a nickel-based catalyst bed from top to bottom, and are subjected to catalytic reaction under the pressure of 1-12 MPa and the temperature of 250-500 ℃ to obtain the first post-tower gas; and/or the number of the groups of groups,
the synthesis gas and the first tower post gas enter from the top of the second synthesis equipment, pass through a nickel-based catalyst bed layer from top to bottom, and are subjected to catalytic reaction at the pressure of 1-12 MPa and the temperature of 250-550 ℃ to obtain the second tower post gas; and/or the number of the groups of groups,
the recycle gas enters from the top of the third synthesis equipment, passes through a nickel-based catalyst bed layer from top to bottom, and undergoes catalytic reaction at the pressure of 1-12 MPa and the temperature of 250-300 ℃ to obtain the primary methane.
In one embodiment, the space velocity of the recycle gas entering the third synthesis device is less than the space velocity of the synthesis gas and the first post-column gas entering the second synthesis device, the space velocity of the recycle gas entering the third synthesis device is less than the space velocity of the synthesis gas and the recycle gas entering the first synthesis device, and the space velocity of the synthesis gas and the recycle gas entering the first synthesis device is greater than or equal to the space velocity of the synthesis gas and the first post-column gas entering the second synthesis device.
According to the technical scheme, the invention has the advantages and positive effects that:
the first synthesis equipment, the second synthesis equipment and the third synthesis equipment are allocated in series and in parallel to ensure that the reaction balance of the synthesis gas is more thorough, the single-pass methane conversion rate can be obtained to the greatest extent, the compression power consumption is low, the energy heat recovery is concentrated, and the energy consumption of the whole methane preparation system is reduced.
The methane preparation method has the advantages of high conversion rate, small circulation, flexible and controllable temperature of methanation synthesis equipment, wide capacity adjustment range, more reasonable system heat exchange, lower energy consumption, high energy heat recovery and high product steam quality.
Drawings
FIG. 1 is a schematic diagram of a system for producing liquid carbon dioxide in accordance with the present invention.
The reference numerals are explained as follows:
1. a first heat exchange device; 2. a first synthesizing device; 3. a second synthesizing device; 4. a second heat exchange device; 5. a gas-liquid separation device; 6. a supercharging device; 7. a third synthesizing device; 8. a first flow regulating valve; 9. a steam superheater; 10. a steam regulating valve; 11. a second flow regulating valve; 12. a first steam generator; 13. a first cooling device; 14. a second steam generator; 15. a gas-liquid separator; 16. and a second cooling device.
Detailed Description
Exemplary embodiments that embody features and advantages of the present invention will be described in detail in the following description. It will be understood that the invention is capable of various modifications in various embodiments, all without departing from the scope of the invention, and that the description and illustrations herein are intended to be by way of illustration only and not to be construed as limiting the invention.
For the purpose of further illustrating the principles and structure of the present invention, preferred embodiments of the invention will now be described in detail with reference to the accompanying drawings.
The synthesis reaction equation of methane is as follows:
CO+3H 2 ＝CH 4 CO 2 +4H 2 ＝CH 4 +2H 2 O。
the synthesis reaction of methane is exothermic, and H can be increased at low temperature 2 Probability of methane synthesis. Thus, the lower the temperature, the synthesis goes towards CH 4 The more the direction moves.
The invention provides a methane preparation system which can be used for synthesizing methane by controlling the temperature of synthesis gas containing hydrogen, carbon monoxide and carbon dioxide, and has low energy consumption.
Fig. 1 shows a schematic diagram of a methane production system, referring to fig. 1, comprising a first heat exchange device 1, a first synthesis device 2, a second synthesis device 3, a second heat exchange device 4, a gas-liquid separation device 5, a pressure boosting device 6, a third synthesis device 7, and a cooling and separation device.
The first heat exchange device 1 comprises a first heat channel and a first medium channel which are independent of each other and are capable of heat exchange. The inlet of the first medium channel is used for receiving outside synthesis gas, namely, the inlet of the first medium channel is used for communicating with the outside.
Wherein the main component of the synthesis gas is hydrogen (H 2 ) Carbon monoxide (CO) and carbon dioxide (CO) 2 ). In the synthesis gas (H) used in the present application 2 -CO 2 )/(CO+CO 2 ) Is greater than 3 volume percent, i.e., the hydrogen content of the synthesis gas is such that it is sufficient and abundant to react with carbon monoxide and carbon dioxide, depending on the methane synthesis reaction.
The synthesis gas undergoes heat exchange in the first heat exchange device 1, and the synthesis gas absorbs heat and rises in temperature.
The first synthesis device 2 is connected to the outlet of the first medium channel to receive the warmed synthesis gas. The first synthesis apparatus 2 is used for methane synthesis reaction to obtain a first post-tower gas. Wherein in the first synthesis plant 2, the synthesis gas undergoes a methane synthesis reaction when the recycle gas has not yet been produced. After the recycle gas enters the first synthesis apparatus 2, the synthesis gas and the recycle gas are subjected to a methane synthesis reaction together.
Specifically, the first synthesis apparatus 2 is an adiabatic synthesis reactor in the axial and radial direction. The first synthesis apparatus 2 is packed with a nickel catalyst. The first synthesizing device 2 adopts a separated design of a shell and an internal part, the shell bears external pressure, the temperature is consistent with the air inlet temperature, and the material is saved. The internal parts bear the gas distribution function and the heat of reaction of the catalyst, but do not bear pressure. The overall structure of the first synthesizing device 2 is safe and reliable.
The outlet of the first synthesis device 2 communicates with the inlet of the first heat channel to deliver the first column off-gas. Namely, in the first heat exchange device 1, the first post-tower gas exchanges heat with the synthesis gas, the first post-tower gas releases heat to cool, and the synthesis gas absorbs heat to heat.
Further, a first flow regulating valve 8 is provided between the first medium channel and the first synthesizing device 2. The opening of the first flow regulating valve 8 is adjustable and thereby the amount of synthesis gas entering the first synthesis plant 2. By adjusting the amount of synthesis gas entering the first synthesis device 2, the volume percentage of synthesis gas and total carbon oxides in the recycle gas in the first synthesis device 2 is adjusted, and thus the reaction degree of methane synthesis is adjusted, so that the temperature rise in the first synthesis device 2 can be controlled.
Preferably, a steam superheater 9 is also provided between the first synthesis apparatus 2 and the first heat channel. The steam superheater 9 comprises a heating conduit in which steam is passed, the steam absorbing heat from the first column post gas to form superheated steam. In this embodiment, a cylinder is disposed outside the heating pipe, and a space for the first post-tower gas to pass through is provided between the cylinder and the heating pipe, i.e. the first post-tower gas passes through outside the heating pipe and provides heat to the steam.
The outlet of the heating pipe communicates with the inlet of the second synthesis apparatus 3 to feed superheated steam to the second synthesis apparatus 3.
Specifically, a steam regulating valve 10 is also provided between the steam superheater 9 and the second synthesis apparatus 3, i.e. the steam regulating valve 10 is arranged between the heating pipe and the second synthesis apparatus 3 to regulate the amount of superheated steam entering the second synthesis apparatus 3.
The inlet of the second synthesis device 3 is connected to both the outlet of the first medium channel and the outlet of the first heat channel for receiving the warmed synthesis gas and the cooled first post-tower gas.
And the heated synthesis gas and the cooled first post-tower gas react in the second synthesis equipment 3 to obtain second post-tower gas.
When the methane synthesis reaction occurs in the second synthesis device 3, the speed of the methane synthesis reaction is controlled by introducing superheated steam, so that the reaction is prevented from being too fast. And the entry of superheated steam also reduces the temperature rise in the whole second synthesis plant 3.
Specifically, the second synthesis apparatus 3 is an adiabatic synthesis reactor in the axial-radial direction. The second synthesis apparatus 3 is packed with a nickel catalyst. The second synthesizing device 3 adopts a separated design of a shell and an internal part, the shell bears external pressure, the temperature is consistent with the air inlet temperature, and the material is saved. The internal parts bear the gas distribution function and the heat of reaction of the catalyst, but do not bear pressure. The second synthesizing device 3 is safe and reliable in overall structure.
Further, a second flow regulating valve 11 is provided between the second synthesizing apparatus 3 and the first medium passage. The opening of the second flow regulating valve 11 is adjustable and thereby the amount of synthesis gas entering the second synthesis plant 3.
The second heat exchange device 4 includes a second heat channel and a second medium channel which are independent of each other and are capable of heat exchange. The inlet of the second heat channel is connected with the second synthesis device 3 to receive the second post-tower gas, i.e. the second post-tower gas releases heat to cool. The outlet of the second medium channel is in communication with the inlet of the first synthesis device 2.
Further, a first steam generator 12 is also provided between the second synthesis device 3 and the second heat exchange device 4. Specifically, the first steam generator 12 is connected to the inlet of the second heat path. The first steam generator 12 comprises a first water supply conduit for water circulation, and the second post-tower gas is used for providing heat to the water in the first water supply conduit to convert the water into steam, and an outlet of the first water supply conduit is communicated with a heating conduit of the steam superheater 9.
The water inlet of the first water supply pipeline is used for being communicated with the outside. In this embodiment, the water of the first water supply line is boiler water.
The water is converted into steam by absorbing heat after entering the first water supply pipeline, and then enters the steam superheater 9 to be converted into superheated steam which enters the second synthesis equipment 3.
The gas-liquid separation device 5 is arranged at the downstream of the second heat channel to receive the cooled second post-tower gas and perform gas-liquid separation to separate water.
Further, a first cooling device 13 is provided between the second heat exchange device 4 and the gas-liquid separation device 5. The first cooling device 13 is used for further cooling the second column off-gas. In this embodiment, the first cooling device 13 may be a circulating water cooling device or a desalted water heat exchanging device.
Specifically, the temperature of the second post-tower gas after passing through the first evaporator, the second heat exchange device 4 and the first cooling device 13 is reduced to 30-80 ℃.
The pressurizing device 6 is arranged downstream of the gas-liquid separation device 5 to receive the second post-tower gas after separating water and pressurize the second post-tower gas to obtain circulating gas. In this embodiment, the pressurizing device 6 is a circulator.
The pressurizing device 6 is in communication with the inlet of the second medium channel, i.e. delivers the circulating gas to the second medium channel of the second heat exchange device 4. The circulating gas exchanges heat with the second post-tower gas in the second heat exchange equipment 4, the circulating gas absorbs heat to raise the temperature, and the second post-tower gas releases heat to lower the temperature.
A third synthesis device 7 is arranged in parallel with the first synthesis device 2 downstream of the second medium channel to receive the recycle gas and to provide the recycle gas for methane synthesis reactions.
Specifically, the third synthesis apparatus 7 is an adiabatic synthesis reactor in the axial and radial direction. The third synthesis apparatus 7 is packed with a nickel catalyst. The third synthesizing device 7 adopts a separated design of a shell and an internal part, the shell bears external pressure, the temperature is consistent with the air inlet temperature, and the material is saved. The internal parts bear the gas distribution function and the heat of reaction of the catalyst, but do not bear pressure. The third synthesizing device 7 is safe and reliable in overall structure.
The cooling and separating device is arranged at the downstream of the third synthesizing device 7 to receive the synthesized primary methane and cool the primary methane and separate the gas from the liquid to obtain methane products.
Specifically, the cooling and separating apparatus includes a second steam generator 14 and a gas-liquid separator 15.
The second steam generator 14 includes a second water feed line for water circulation, and the primary methane is used to provide heat to the water in the second water feed line to convert the water to steam, and the primary methane is cooled after releasing the heat.
In particular, the second steam generator 14 is connected to the outlet of the third synthesis apparatus 7 to receive preliminary methane.
The outlet of the second water supply pipeline outputs low-pressure saturated steam which can be stored and utilized or sold.
The gas-liquid separator 15 is used to separate water from the primary methane.
Further, a second cooling device 16 is provided between the second steam generator 14 and the gas-liquid separator 15.
Specifically, the primary methane is cooled by the second steam generator 14 and the second cooling device 16, then the temperature is reduced to 30-50 ℃, and the methane product is output after being separated by the gas-liquid separator 15.
In the methane production system of the present embodiment, the first heat exchange device, the first synthesis device 2, the second synthesis device 3, the second heat exchange device 4, the steam superheater 9, the first steam generator 12, the first cooling device 13, and the gas-liquid separation device 5 form an open circulation loop.
In the open circulation loop, the first synthesis equipment 2 and the second synthesis equipment 3 exist in a serial connection mode and also exist in a parallel connection mode, wherein when synthesis gas is divided into two paths and respectively enters the first synthesis equipment 2 and the second synthesis equipment 3, the two paths are in parallel connection, and when the first tower post gas enters the second synthesis equipment 3 after being cooled, the two paths are in serial connection.
The first synthesis equipment 2 and the second synthesis equipment 3 are connected in series and in parallel, so that the distribution of synthesis gas flow and the design of overheat steam control temperature rise ensure proper reaction temperature, and meanwhile, higher conversion rate and stable operation characteristic are realized.
In the above-described open circulation loop, the first synthesis apparatus 2 is an auxiliary reactor and the second synthesis apparatus 3 is a main reactor. Wherein the second synthesis plant 3 is a plant for production regulation of the whole methane production system, in particular the capacity and the recycle ratio of the whole production system are regulated by regulating the amount of superheated steam entering the second synthesis plant 3. Therefore, the whole methane preparation system has large capacity control and adjustment range and strong adaptability.
The third synthesis apparatus 7 is connected in series with the open circulation loop and receives the recycle gas, so that the third synthesis apparatus 7 mainly carries out deep purification reaction, the reaction temperature is close to constant temperature, and the produced primary methane has almost no carbon oxides.
After the synthesis gas has passed through the first synthesis device 2 and the second synthesis device 3, the carbon oxides (co+co) 2 ) The higher consumption of the carbon oxides in the second column off-gas formed is lower. After the recycle gas has passed through the third synthesis unit 7, the carbon oxides (CO+CO 2 ) Is deeply purified, i.e. the primary methane formed is almost free of carbon oxides.
The series and parallel flow allocation ensures that the reaction balance of the synthesis gas is more thorough, the single-pass methane conversion rate can be obtained to the greatest extent, the compression power consumption is low, the energy heat recovery is more concentrated, the byproduct steam is higher in quality, the recovery amount is high, and the method is more economical.
The invention also provides a preparation method of methane, which comprises the following steps:
s1, providing synthesis gas, (H) 2 -CO 2 )/(CO+CO 2 ) Is greater than 3 volume percent.
The synthesis gas may be obtained by gasification of biomass itself or may be obtained by outsourcing.
The synthesis gas is in a surplus state in the methane synthesis reaction by the amount of hydrogen in the synthesis gas, namely, when carbon monoxide and carbon dioxide react with hydrogen, the amount of hydrogen can ensure that the carbon monoxide and the carbon dioxide completely react to generate methane according to theoretical calculation.
S2, the synthesis gas is heated through heat exchange and then enters the first synthesis equipment 2 and the second synthesis equipment 3 respectively.
The synthesis gas is split into two paths which enter the first synthesis apparatus 2 and the second synthesis apparatus 3 respectively, at which point the first synthesis apparatus 2 and the second synthesis apparatus 3 may be understood as being arranged in parallel.
Preferably, the amount of synthesis gas entering the first synthesis device 2 can be adjusted. The amount of synthesis gas entering the first synthesis device 2 is adjusted such that the molar percentage of synthesis gas in the first synthesis device 2 to total carbon oxides in the recycle gas is 3.0-5.0%. Specifically, a first flow regulating valve 8 is provided between the first synthesis device 2 and the first heat exchange device 1, and the amount of synthesis gas entering the first synthesis device 2 is achieved by the regulation of this first flow regulating valve 8.
Further, the amount of synthesis gas entering the second synthesis device 3 is also adjusted such that the molar percentage of synthesis gas in the second synthesis device 3 to total carbon oxides in the second column post gas is 3.0-10.0%.
In particular, a second flow regulating valve 11 is provided between the second synthesis device 3 and the first heat exchange device 1, by means of which second flow regulating valve 11 the amount of synthesis gas entering the second synthesis device 3 is achieved.
S3, methane synthesis reaction is carried out in the first synthesis equipment 2 to obtain first tower post gas.
Specifically, synthesis gas and recycle gas generated subsequently enter from the top of the first synthesis equipment 2, pass through a nickel-based catalyst bed layer from top to bottom, and undergo catalytic reaction at the pressure of 1-12 MPa and the temperature of 250-500 ℃ to obtain first tower post gas.
Wherein 75-85% of the carbon oxides are catalytically converted to methane in the first synthesis apparatus 2.
Part of the heat of reaction generated by the methane synthesis reaction in the first synthesis apparatus 2 enters the steam superheater 9, and the heat is released to steam, and the other part is integrated into the recycle gas.
S4, cooling the first post-tower gas and the synthesis gas through heat exchange, and then entering the second synthesis equipment 3, wherein the first post-tower gas and the synthesis gas jointly perform methane synthesis reaction in the second synthesis equipment 3 to obtain the second post-tower gas.
Specifically, the synthesis gas and the first post-tower gas enter from the top of the second synthesis equipment 3, pass through a nickel-based catalyst bed from top to bottom, and undergo catalytic reaction at the pressure of 1-12 MPa and the temperature of 250-550 ℃ to obtain the second post-tower gas.
Further, before the heat exchange between the first post-tower gas and the synthesis gas, the method further comprises the following steps:
the first post-tower gas exchanges heat with steam, releases heat to convert the steam into superheated steam, exchanges heat with the synthesis gas after cooling, and enters the second synthesis device 3.
S5, cooling the second tower gas, and then performing gas-liquid separation to separate water from the second tower gas.
S6, pressurizing the second tower post gas after water separation to form circulating gas, carrying out heat exchange and heating on the circulating gas and the second tower post gas, and then entering the first synthesis equipment 2 and the third synthesis equipment 7, and carrying out methane synthesis reaction in the third synthesis equipment 7 to obtain primary methane.
Specifically, the recycle gas and the synthesis gas enter from the top of the third synthesis equipment 7, pass through a nickel-based catalyst bed layer from top to bottom, and undergo catalytic reaction at the pressure of 1-12 MPa and the temperature of 250-300 ℃ to obtain primary methane.
S7, cooling and gas-liquid separation are carried out on the primary methane to obtain the product methane.
In the above preparation method, the space velocity of the recycle gas entering the third synthesis apparatus 7 is controlled to be smaller than the space velocity of the synthesis gas and the first post-tower gas entering the second synthesis apparatus 3, the space velocity of the recycle gas entering the third synthesis apparatus 7 is controlled to be smaller than the space velocity of the synthesis gas and the recycle gas entering the first synthesis apparatus 2, and the space velocity of the synthesis gas and the recycle gas entering the first synthesis apparatus 2 is controlled to be larger than or equal to the space velocity of the synthesis gas and the first post-tower gas entering the second synthesis apparatus 3.
Wherein the space velocity of each synthesis device is realized by controlling the loading of the catalyst. Specifically, by controlling the catalyst loading, gas is directed through the catalyst bed at a desired space velocity.
In the preparation method of methane, the airspeed and larger ventilation in the first synthesis equipment 2 and the second synthesis equipment 3 can effectively avoid the local heat accumulation phenomenon of the catalyst bed, are beneficial to reducing the temperature of a catalytic reaction hot spot, slow down excessive heat release of the methane catalyst in a local area under high hydrogen and high carbon partial pressure, and enable more than 80-90% of reaction areas of the catalyst bed to be in a high-temperature (350-550 ℃) and high-conversion reaction temperature area, so that the overall service efficiency and service life of the catalyst are improved.
The space velocity in the third synthesis equipment 7 is lower, the reaction bed temperature is more uniform due to the low space velocity and low carbon partial pressure, the catalyst bed is in a reaction temperature zone with high conversion depth at the low temperature of 250-300 ℃, the improvement of the single-pass conversion rate of the synthesis loop is facilitated, and the requirement of deep purification of methane gas is met.
In the first synthesis plant 2, synthesis gas and recycle gas are fed at high space velocity, suitable carbon oxygen compounds (co+co 2 ) The catalyst reacts at the content of 3.0-5.0 percent so that the catalyst does not generate local overtemperature. In the second synthesis apparatus 3, the synthesis gas and the first column post gas are fed with superheated steam at a higher space velocity, and the carbon oxides (co+co 2 ) The catalyst is reacted under the condition of the content (3.0-10%), and the temperature rise of a reaction bed layer and the single-pass methane yield are controlled, so that the catalyst does not generate local overtemperature.
The methane preparation method has the advantages of high conversion rate, small circulation, flexible and controllable methanation synthesis equipment temperature, large capacity adjustment range, more reasonable system heat exchange, lower energy consumption, high energy heat recovery and high product steam quality.
While the invention has been described with reference to several exemplary embodiments, it is to be understood that the terminology used is intended to be in the nature of words of description and of limitation. As the present invention may be embodied in several forms without departing from the spirit or essential characteristics thereof, it should also be understood that the above-described embodiments are not limited by any of the details of the foregoing description, but rather should be construed broadly within its spirit and scope as defined in the appended claims, and therefore all changes and modifications that fall within the meets and bounds of the claims, or equivalences of such meets and bounds are therefore intended to be embraced by the appended claims.
Claims (15)
1. A methane production system, comprising:
a first heat exchange device including a first heat channel and a first medium channel which are independent of each other and capable of heat exchange; the inlet of the first medium channel is used for receiving outside synthesis gas, and the inlet of the first medium channel is used for receiving outside synthesis gas (H 2 -CO 2 )/(CO+CO 2 ) Is greater than 3 volume percent;
a first synthesizing device connected to an outlet of the first medium channel; the first synthesis equipment is used for carrying out methane synthesis reaction to obtain first tower post gas; the outlet of the first synthesis device communicates with the inlet of the first heat channel to provide the first column off-gas;
the inlet of the second synthesis equipment is connected with the outlet of the first medium channel and the outlet of the first heat channel at the same time and is used for receiving the synthesis gas after temperature rise and the first tower post gas after temperature reduction; the second synthesis equipment is used for carrying out methane synthesis reaction to obtain second tower post gas;
a second heat exchange device including a second heat channel and a second medium channel which are independent of each other and capable of heat exchange; the inlet of the second heat channel is connected with the second synthesis equipment to receive the second post-tower gas; the outlet of the second medium channel is communicated with the inlet of the first synthesis equipment;
the gas-liquid separation device is arranged at the downstream of the second heat channel and used for receiving the cooled second tower post gas and performing gas-liquid separation to separate water;
the pressurizing device is arranged at the downstream of the gas-liquid separation device and is used for receiving the second tower post gas after water is separated and pressurizing to obtain circulating gas, and the pressurizing device is communicated with the inlet of the second medium channel;
a third synthesis device disposed in parallel with the first synthesis device and downstream of the second media path to receive the recycle gas and provide the recycle gas for methane synthesis reactions;
the cooling and separating device is arranged at the downstream of the third synthesizing device to receive the synthesized primary methane and cool the primary methane and separate gas from liquid to obtain a methane product.
2. The methane production system of claim 1, wherein a first flow regulating valve is disposed between the first media channel and the first synthesis device; and/or the number of the groups of groups,
and a second flow regulating valve is arranged between the first medium channel and the second synthesizing equipment.
3. The methane production system of claim 1, wherein a steam superheater is further disposed between the first synthesis plant and the first heat channel, the steam superheater comprising a heating conduit for passing steam inside, the steam absorbing heat from the first post-column gas to form superheated steam, an outlet of the heating conduit communicating with an inlet of the second synthesis plant to input the superheated steam to the second synthesis plant.
4. A methane production system according to claim 3, wherein a first steam generator is further provided between the second synthesis plant and the second heat exchange plant, the first steam generator comprising a first feed water conduit for water circulation, the second post-column gas being adapted to provide heat to water in the first feed water conduit for conversion of water to steam, the outlet of the first feed water conduit being in communication with the heating conduit of the steam superheater.
5. The methane production system according to claim 1, wherein a first cooling device is further provided between the second heat exchange device and the gas-liquid separation device.
6. The methane production system of claim 1, wherein the cooling and separation apparatus comprises a second steam generator and a gas-liquid separator;
the second steam generator comprises a second water supply pipeline for water supply circulation, the primary methane is used for providing heat for water in the second water supply pipeline so as to enable the water to be converted into steam, and the gas-liquid separator is used for receiving the primary methane after temperature reduction and performing gas-liquid separation to obtain methane products.
7. The methane production system of claim 6, wherein a second cooling device is further disposed between the second steam generator and the gas-liquid separator.
8. The methane production system of claim 1, wherein the first synthesis apparatus is charged with a nickel catalyst, the second synthesis apparatus is charged with a nickel catalyst, and the third synthesis apparatus is charged with a nickel catalyst.
9. The methane production system of claim 1, wherein the first synthesis apparatus, the second synthesis apparatus, and the third synthesis apparatus are all shaft radial adiabatic synthesis reactors.
10. A method for producing methane, comprising the steps of:
providing synthesis gas, wherein (H) 2 -CO 2 )/(CO+CO 2 ) Is greater than 3 volume percent;
the synthesis gas is heated by heat exchange and then enters into first synthesis equipment and second synthesis equipment respectively;
methane synthesis reaction is carried out in the first synthesis equipment to obtain first tower post gas;
the first post-tower gas and the synthesis gas enter the second synthesis equipment after heat exchange and temperature reduction, and the first post-tower gas and the synthesis gas jointly perform methane synthesis reaction in the second synthesis equipment to obtain second post-tower gas;
cooling the second tower post gas, and then performing gas-liquid separation to separate water from the second tower post gas;
pressurizing the second tower gas after water separation to form circulating gas, carrying out heat exchange and heating on the circulating gas and the second tower gas, and then entering the first synthesis equipment and the third synthesis equipment, and carrying out methane synthesis reaction in the third synthesis equipment to obtain primary methane;
and cooling and gas-liquid separating the primary methane to obtain the product methane.
11. The method for producing methane according to claim 10, further comprising the steps of:
adjusting the amount of the synthesis gas entering the first synthesis equipment to make the mole percentage of the total carbon oxides in the synthesis gas and the recycle gas in the first synthesis equipment be 3.0-5.0%; and/or the number of the groups of groups,
the amount of the synthesis gas entering the second synthesis equipment is regulated so that the mole percentage of the total carbon oxides in the synthesis gas and the second post-tower gas in the second synthesis equipment is 3.0-10.0%.
12. The method for producing methane according to claim 10, further comprising the steps of, before the second post-column gas exchanges heat with the recycle gas:
and the second post-tower gas exchanges heat with water, releases heat to convert the water into steam, exchanges heat with the circulating gas after cooling, and exchanges heat with the first post-tower gas.
13. The method of producing methane according to claim 12, further comprising the steps of, before the first post-column gas exchanges heat with the synthesis gas:
and the first post-tower gas exchanges heat with the steam, releases heat to convert the steam into superheated steam, and the superheated steam enters the second synthesis equipment, and exchanges heat with the synthesis gas.
14. The method for producing methane according to claim 10, wherein the synthesis gas and the recycle gas enter from the top of the first synthesis equipment and pass through a nickel-based catalyst bed from top to bottom, and are subjected to catalytic reaction at a pressure of 1 to 12MPa and a temperature of 250 to 500 ℃ to obtain the first post-tower gas; and/or the number of the groups of groups,
the synthesis gas and the first tower post gas enter from the top of the second synthesis equipment, pass through a nickel-based catalyst bed layer from top to bottom, and are subjected to catalytic reaction at the pressure of 1-12 MPa and the temperature of 250-550 ℃ to obtain the second tower post gas; and/or the number of the groups of groups,
the recycle gas enters from the top of the third synthesis equipment, passes through a nickel-based catalyst bed layer from top to bottom, and undergoes catalytic reaction at the pressure of 1-12 MPa and the temperature of 250-300 ℃ to obtain the primary methane.
15. The method of producing methane according to claim 10, wherein the space velocity of the recycle gas entering the third synthesis apparatus is less than the space velocity of the synthesis gas and the first post-column gas entering the second synthesis apparatus, the space velocity of the recycle gas entering the third synthesis apparatus is less than the space velocity of the synthesis gas and the recycle gas entering the first synthesis apparatus, and the space velocity of the synthesis gas and the recycle gas entering the first synthesis apparatus is greater than or equal to the space velocity of the synthesis gas and the first post-column gas entering the second synthesis apparatus.
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