CN113148952A - System for preparing synthesis gas and hydrogen fuel by methane dry reforming - Google Patents
System for preparing synthesis gas and hydrogen fuel by methane dry reforming Download PDFInfo
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- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
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- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/48—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents followed by reaction of water vapour with carbon monoxide
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- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
- C01B3/56—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
- C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
- C01B2203/0238—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a carbon dioxide reforming step
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0283—Processes for making hydrogen or synthesis gas containing a CO-shift step, i.e. a water gas shift step
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/042—Purification by adsorption on solids
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- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0465—Composition of the impurity
- C01B2203/0475—Composition of the impurity the impurity being carbon dioxide
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- C01B2203/08—Methods of heating or cooling
- C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
- C01B2203/0866—Methods of heating the process for making hydrogen or synthesis gas by combination of different heating methods
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- C01B2203/0872—Methods of cooling
- C01B2203/0883—Methods of cooling by indirect heat exchange
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
- C01B2203/1205—Composition of the feed
- C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
- C01B2203/1235—Hydrocarbons
- C01B2203/1241—Natural gas or methane
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
- C01B2203/1288—Evaporation of one or more of the different feed components
- C01B2203/1294—Evaporation by heat exchange with hot process stream
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
Abstract
The invention discloses a system for preparing synthesis gas and hydrogen fuel by dry reforming of methane, which comprises a high-temperature dry reforming reactor, a solar heat collector, a gas-gas heat exchanger, an intermediate-temperature shift reactor, a low-pressure steam generator, a water supply deaerator and a pressure swing adsorber which are connected through pipelines. The carbon dioxide separated by the pressure swing absorber is injected back into the high-temperature dry reforming reactor, so that the molar quantity of the carbon dioxide in the reactor is several times higher than that of methane, the conversion rate of methane in the methane is improved to the maximum extent, carbon deposit formed by high-temperature cracking of the methane is avoided, and the service lives of the reactor and the catalyst are prolonged. The invention completely recovers the carbon dioxide generated in the hydrogen production process and converts the carbon dioxide into the synthesis gas, can simultaneously output two products of hydrogen fuel and synthesis gas fuel, realizes zero emission of the carbon dioxide of the system, and has the advantages of simple structure, low production cost, long service life, environmental friendliness and the like.
Description
Technical Field
The invention belongs to the technical field of methane utilization, and particularly relates to a system for preparing synthesis gas and hydrogen fuel by dry reforming of methane.
Background
China has abundant biomass resources, and the biological methane becomes an important way for biomass utilization. At present, the methane utilization technology in China is relatively lagged behind, and the problem of low methane utilization efficiency still exists. The hydrogen fuel with high heat value and no pollution is obtained by reforming the methane to prepare the hydrogen, which is the most ideal technical means for upgrading the methane. The main components of the methane are 50-80% of methane and 20-40% of carbon dioxide, so that the methane conversion rate is low when the methane and carbon dioxide dry reforming reaction is carried out on the methane, and meanwhile, the reforming reaction is a strong endothermic reaction and needs to be carried out at a high temperature of more than 645 ℃ and under the action of a catalyst, the unconverted methane is easy to generate a cracking reaction at the high temperature to cause carbon deposition on the surface of the catalyst, the carbon deposition causes the catalyst to lose activity, and even blocks a reaction tube, so that the service life of the reactor is shortened, and the cost of the catalyst is increased. In order to solve the problem, a currently available method is to add steam into the reforming reactor to perform a wet reforming reaction between unconverted methane and the steam, so as to reduce and inhibit the generation of carbon deposit, but the steam is heated to a high temperature in the reforming reactor, so that a large amount of heat energy is consumed, and the requirement on water quality is high, so that the energy consumption and the operation cost of the system are increased. In addition, a large amount of carbon dioxide generated in the traditional methane hydrogen production process can cause greenhouse effect if the carbon dioxide is directly discharged, so that the resource utilization of the carbon dioxide needs to be considered, the complexity of the system is increased, and the popularization and application of the methane reforming hydrogen production technology are restricted. Aiming at the analysis, the invention mainly solves the problems of improving the methane conversion rate, reducing the carbon deposit of the reactor and reducing the energy consumption and the operation cost of the system, and finds a new way for recycling the carbon dioxide.
Disclosure of Invention
The invention aims to provide a system for preparing synthesis gas and hydrogen fuel by dry reforming of methane, which has the advantages of simple structure, low production cost, long service life, environmental friendliness and difficult carbon accumulation.
The purpose of the invention is realized by the following technical scheme:
the invention relates to a system for preparing synthesis gas and hydrogen fuel by dry reforming of methane, which comprises a high-temperature dry reforming reactor, a solar heat collector, a gas-gas heat exchanger, an intermediate-temperature shift reactor, a low-pressure steam generator, a water supply deaerator, a pressure swing adsorber, a methane input pipeline, a carbon dioxide reinjection pipeline, a synthesis gas output pipeline, a shift gas pipeline, a hydrogen output pipeline, a water supply pipeline, a water pipeline deaerating pipeline and a steam pipeline;
a raw material inlet of the high-temperature dry reforming reactor is connected with a methane input pipeline and a carbon dioxide reinjection pipeline, and a synthesis gas outlet of the high-temperature dry reforming reactor is connected with a synthesis gas pipeline; the solar heat collector and the high-temperature dry reforming reactor are used for heat transfer; the synthesis gas pipeline is spirally or zigzag passed through the gas-gas heat exchanger and then divided into two paths: one path is connected with a synthesis gas inlet of the medium temperature shift reactor, the other path is connected with a synthesis gas output pipeline, and a low-pressure steam generator is arranged on the pipeline; the shift gas outlet of the medium temperature shift reactor is connected with the hydrogen output pipeline through a shift gas pipeline, and a water supply deaerator and a pressure swing absorber are sequentially arranged on the shift gas pipeline; a water vapor outlet of the low-pressure steam generator is connected with a synthesis gas inlet of the medium-temperature shift reactor; a water supply inlet of the water supply deaerator is connected with a water supply pipeline, and a deaerated water outlet of the water supply deaerator is connected with a deaerated water inlet of the low-pressure water steam generator through a deaerated water pipeline; the carbon dioxide outlet of the pressure swing adsorber is connected with the front section of the carbon dioxide reinjection pipeline; the front section of the carbon dioxide reinjection pipeline is communicated with the shell side of the gas-gas heat exchanger, and the shell side of the gas-gas heat exchanger is connected with the raw material inlet of the high-temperature dry reforming reactor through the rear section of the carbon dioxide reinjection pipeline.
After the scheme is adopted, the invention has the following advantages:
1) the methane conversion rate of the methane is improved. The carbon dioxide separated by the pressure swing adsorber of the invention exchanges heat through gas and gas
The preheated reactor is injected back into the reforming reactor, so that the molar weight of carbon dioxide in the reactor is several times higher than that of methane, thereby improving the methane conversion rate to the maximum extent.
2) Reduce carbon deposit in the reactor. Because the excessive carbon dioxide gas is reinjected into the reforming reactor of the invention
The carbon dioxide gas and the methane gas are well mixed, so that the methane is prevented from being subjected to pyrolysis to form carbon deposit. On the other hand, carbon dioxide can directly react with the generated carbon deposit to generate carbon monoxide, thereby prolonging the service life of the reactor and the catalyst.
3) Realizing zero emission of carbon dioxide in the hydrogen production process. Because the invention completely recovers the dioxide separated from hydrogen production
Carbon is injected back into the reforming reaction to be converted into synthesis gas, so that the hydrogen fuel is prepared by zero-emission carbon dioxide.
4) The water cost is saved. Because the invention adopts a method of introducing water vapor into the medium-temperature shift reactor, the method is not a method of transferring
The method for introducing the steam into the high-temperature reforming reactor adopted by the traditional technology has the advantages that the temperature of the steam in the reactor is lower, the requirement on water quality is reduced, the water treatment cost is reduced, and the water cost is saved.
5) Improving the thermal economy of the system. In the traditional technology, water vapor is introduced into a high-temperature reforming reactor to generate strong endothermic reaction,
the large heat exchange temperature difference between the water vapor and the heat source greatly reduces the utilization of the available energy. The invention leads the water vapor to the intermediate temperature shift reactor to generate exothermic reaction without heat source, thereby reducing the available energy loss of the system and improving the heat economy of the system.
6) Energy is used in a cascade mode. The invention recovers the high-temperature waste heat of the synthesis gas firstly for preheating the carbon dioxide and then returning the carbon dioxide
The medium-temperature waste heat of the received part of the synthesis gas is used for producing water vapor, and the medium-low temperature waste heat of the converted gas is recovered for supplying water and removing oxygen, so that the energy of the whole system is optimally utilized.
7) Realizing the co-production of multiple products. Because the invention outputs two products of hydrogen fuel and synthesis gas fuel at the same time, the application range is wider, and the comprehensive economic benefit is higher.
Drawings
FIG. 1 is a schematic diagram of the system architecture of the present invention.
Detailed Description
As shown in fig. 1, the invention relates to a system for preparing synthesis gas and hydrogen fuel by dry reforming of methane, which comprises a high-temperature dry reforming reactor 1, a solar heat collector 2, a gas-gas heat exchanger 3, a medium-temperature shift reactor 4, a low-pressure water vapor generator 5, a water supply deaerator 6, a pressure swing adsorber 7, a methane input pipeline 8, a carbon dioxide reinjection pipeline 9, a synthesis gas pipeline 10, a synthesis gas output pipeline 11, a shift gas pipeline 12, a hydrogen output pipeline 13, a water supply pipeline 14, a deaerated water pipeline 15 and a water vapor pipeline 16.
The raw material inlet of the high-temperature dry reforming reactor 1 is connected with a methane input pipeline 8 and a carbon dioxide reinjection pipeline 9, and the synthesis gas outlet of the high-temperature dry reforming reactor 1 is connected with a synthesis gas pipeline 10; the solar heat collector 2 and the high-temperature dry reforming reactor 1 are in heat transfer; the synthesis gas pipeline 10 is spirally or zigzag passed through the gas-gas heat exchanger 3 and then divided into two paths: one path is connected with a synthesis gas inlet of the medium temperature shift reactor 4, the other path is connected with a synthesis gas output pipeline 11, and a low-pressure water vapor generator 5 is arranged on the pipeline; the shift gas outlet of the medium temperature shift reactor 4 is connected with a hydrogen output pipeline 13 through a shift gas pipeline 12, and a water supply deaerator 6 and a pressure swing absorber 7 are sequentially arranged on the shift gas pipeline 12; a water vapor outlet of the low-pressure steam generator 5 is connected with a synthesis gas inlet of the medium-temperature shift reactor 4; a feed water inlet of the feed water deaerator 6 is connected with a feed water pipeline 14, and a deaerated water outlet of the feed water deaerator 6 is connected with a deaerated water inlet of the low-pressure steam generator 5 through a deaerated water pipeline 15; the carbon dioxide outlet of the pressure swing adsorber 7 is connected with the front section of the carbon dioxide reinjection pipeline 9; the front section of the carbon dioxide reinjection pipeline 9 is communicated with the shell side of the gas-gas heat exchanger 3, and the shell side of the gas-gas heat exchanger 3 is connected with the raw material inlet of the high-temperature dry reforming reactor 2 through the rear section of the carbon dioxide reinjection pipeline 9.
The working principle of the invention is as follows:
the biogas Z raw material from the biogas input pipeline 8 and the carbon dioxide gas from the carbon dioxide reinjection pipeline 9 are mixed and then enter the high-temperature dry reforming reactor 1 to carry out synthetic reaction, the reaction is carried out under the atmosphere of excessive carbon dioxide, and the required heat is provided by the solar heat collector 2. The high-temperature synthesis gas obtained from the high-temperature dry reforming reactor 1 is sent to a gas-gas heat exchanger 3 through a synthesis gas pipeline 10Waste heat recovery is performed for preheating carbon dioxide. The medium-temperature synthesis gas obtained after heat release is divided into two paths: one path enters the medium temperature shift reactor 4 for shift reaction, and the other path is sent to the low pressure steam generator 5 for recycling the waste heat of the synthesis gas for generating the steam H2O, steam H obtained2O is sent into the medium temperature shift reactor 4 through a water vapor pipeline 16, and the synthesis gas H after waste heat recovery is output as a product through a synthesis gas output pipeline 11. The medium temperature shift gas obtained from the medium temperature shift reactor 4 passes through a shift gas pipeline 12, firstly, the heat is released by a water supply deaerator 6 to carry out thermal deoxidization on the water supply G, and then the carbon dioxide CO gas in the shift gas is separated out by a pressure swing absorber 72The deaerated feed water is sent to a low-pressure steam generator 5 through a deaerated water pipeline 15, and the separated high-purity hydrogen H2And is output as a product through a hydrogen output pipeline 13. Carbon dioxide gas CO separated by the pressure swing adsorber 72Is preheated by a gas-gas heat exchanger 3 through a carbon dioxide reinjection pipeline 9 and then is sent to the inlet of the high-temperature dry reforming reactor 1.
The core of the invention is characterized in that: the carbon dioxide separated by the pressure swing absorber 7 is reinjected into the high-temperature dry reforming reactor 1, so that the conversion rate of methane in the methane is improved, the problem of carbon deposition in the reactor is remarkably reduced, and zero emission of the carbon dioxide is really realized.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not intended to limit the present invention in any way, and all simple modifications, equivalent variations and modifications made to the above embodiments according to the technical spirit of the present invention are within the scope of the present invention.
Claims (1)
1. A system for preparing synthesis gas and hydrogen fuel by dry reforming of biogas is characterized in that: the system comprises a high-temperature dry reforming reactor, a solar heat collector, a gas-gas heat exchanger, a medium-temperature shift reactor, a low-pressure steam generator, a water supply deaerator, a pressure swing adsorber, a methane input pipeline, a carbon dioxide reinjection pipeline, a synthetic gas output pipeline, a shift gas pipeline, a hydrogen output pipeline, a water supply pipeline, a deaerating water pipeline and a steam pipeline;
a raw material inlet of the high-temperature dry reforming reactor is connected with a methane input pipeline and a carbon dioxide reinjection pipeline, and a synthesis gas outlet of the high-temperature dry reforming reactor is connected with a synthesis gas pipeline; the solar heat collector and the high-temperature dry reforming reactor are used for heat transfer; the synthesis gas pipeline is spirally or zigzag passed through the gas-gas heat exchanger and then divided into two paths: one path is connected with a synthesis gas inlet of the medium temperature shift reactor, the other path is connected with a synthesis gas output pipeline, and a low-pressure steam generator is arranged on the pipeline; the shift gas outlet of the medium temperature shift reactor is connected with the hydrogen output pipeline through a shift gas pipeline, and a water supply deaerator and a pressure swing absorber are sequentially arranged on the shift gas pipeline; a water vapor outlet of the low-pressure steam generator is connected with a synthesis gas inlet of the medium-temperature shift reactor; a water supply inlet of the water supply deaerator is connected with a water supply pipeline, and a deaerated water outlet of the water supply deaerator is connected with a deaerated water inlet of the low-pressure water steam generator through a deaerated water pipeline; the carbon dioxide outlet of the pressure swing adsorber is connected with the front section of the carbon dioxide reinjection pipeline; the front section of the carbon dioxide reinjection pipeline is communicated with the shell side of the gas-gas heat exchanger, and the shell side of the gas-gas heat exchanger is connected with the raw material inlet of the high-temperature dry reforming reactor through the rear section of the carbon dioxide reinjection pipeline.
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| CN202110382013.XA CN113148952A (en) | 2021-04-09 | 2021-04-09 | System for preparing synthesis gas and hydrogen fuel by methane dry reforming |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114408867A (en) * | 2021-12-31 | 2022-04-29 | 集美大学 | Hydrogen production system based on methane dry reforming |
| CN114604827A (en) * | 2022-02-28 | 2022-06-10 | 集美大学 | System and method for preparing synthesis gas based on methane dry-wet reforming coupling methanol cracking |
| US20220325950A1 (en) * | 2021-04-07 | 2022-10-13 | Hyundai Motor Company | Lng reforming system and method of controlling the same |
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2021
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20220325950A1 (en) * | 2021-04-07 | 2022-10-13 | Hyundai Motor Company | Lng reforming system and method of controlling the same |
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| CN114604827A (en) * | 2022-02-28 | 2022-06-10 | 集美大学 | System and method for preparing synthesis gas based on methane dry-wet reforming coupling methanol cracking |
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