CN110835094A - Methanol steam and hydrogen mixed gas integrated ultrahigh pressure hydrogen production system and method thereof - Google Patents
Methanol steam and hydrogen mixed gas integrated ultrahigh pressure hydrogen production system and method thereof Download PDFInfo
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Abstract
The invention relates to a methanol steam and hydrogen mixed gas integrated ultrahigh pressure hydrogen production system, which comprises a three-phase heat exchange device, a reforming device, a hydrogen separation device, a steam trap, a water-cooling heat exchanger, a refrigerator and a carbon dioxide liquefaction device, wherein the three-phase heat exchange device is connected with the reforming device; the pump pressure of the liquid pump is 40-100 Mpa, the operation temperature of the water-cooling heat exchanger is less than or equal to 30.8 ℃, and pure hydrogen is sent into the hydrogen storage tank under the pump pressure of the liquid pump; a ultrahigh pressure hydrogen production method comprises the steps of carrying out methanol steam reforming reaction to generate a mixed gas of hydrogen, carbon dioxide and carbon monoxide, then carrying out hydrogen separation, preparing liquid carbon dioxide and hydrogen mixed residual gas in a carbon dioxide separator, wherein the ratio of the liquid carbon dioxide and hydrogen mixed residual gas to the hydrogen, carbon dioxide and carbon monoxide mixed gas is approximate; and the hydrogen and the water enter a hydrogen separation cavity together for hydrogen separation operation. The hydrogen production efficiency of the hydrogen production system is improved, so that the hydrogen production system can be used for manufacturing small-sized hydrogen production equipment.
Description
Technical Field
The invention relates to a methanol steam and hydrogen mixed gas integrated ultrahigh pressure hydrogen production system and a method thereof.
Background
The hydrogen energy is the most ideal energy in the 21 st century, is used as automobile fuel, is easy to start at low temperature, has small corrosion effect on an engine, and can prolong the service life of the engine. Because the hydrogen and the air can be uniformly mixed, a carburetor used on a common automobile can be completely omitted, and the structure of the existing automobile can be simplified. It is more interesting to add only 4% hydrogen to the gasoline. When it is used as fuel of automobile engine, it can save oil by 40%, and has no need of making great improvement on gasoline engine. A hydrogen fuel cell serves as a power generation system.
No pollution, and no pollution to environment caused by fuel cell. It is through electrochemical reaction, rather than combustion (gasoline, diesel) or energy storage (battery) -the most typical traditional backup power scheme. Combustion releases pollutants like COx, NOx, SOx gases and dust. As described above, the fuel cell generates only water and heat. If the hydrogen is generated by renewable energy sources (photovoltaic panels, wind power generation, etc.), the whole cycle is a complete process without generating harmful emissions.
No noise, quiet fuel cell operation, about only 55dB noise, which corresponds to the level of normal human conversation. This makes the fuel cell suitable for a wide range of applications, including indoor installations, or where there is a limit to noise outdoors.
The efficiency is high, the generating efficiency of the fuel cell can reach more than 50%, which is determined by the conversion property of the fuel cell, chemical energy is directly converted into electric energy without intermediate conversion of heat energy and mechanical energy (a generator), and the efficiency is reduced once more because of once more energy conversion.
At present, the main source of hydrogen of a hydrogen energy source hydrogenation station is that an energy storage tank is transported back from outside, and the whole hydrogenation station needs to store a large amount of hydrogen; research finds that hydrogen in the hydrogen energy industry comprises four links, namely hydrogen preparation, hydrogen storage, hydrogen transportation and hydrogen addition (adding hydrogen into a hydrogen energy vehicle), wherein the two links of hydrogen preparation and hydrogen addition are safe at present, accidents easily occur in the hydrogen storage link, and the cost of the hydrogen transportation link is high and is related to the characteristics of hydrogen; the problems of explosion of the hydrogenation station and the reason of high hydrogenation cost frequently occur in the current news.
Therefore, in order to reduce the problem of large amount of hydrogen storage in the existing hydrogen refueling station and shorten or reduce the high cost of the hydrogen transportation link, a hydrogen refueling station system needs to be redesigned.
Disclosure of Invention
The technical problem to be solved by the invention is as follows: the defects of the prior art are overcome, the integrated ultrahigh pressure hydrogen production system of the methanol steam and the hydrogen mixed gas is provided, and the problem that the hydrogen production system is complicated due to the fact that a reformer of the methanol steam and water gas reforming are two independent devices in the prior art is solved;
meanwhile, an ultrahigh pressure hydrogen production method is provided, and the problems that the existing hydrogen production process is complex and the circular hydrogen production cannot be realized are solved.
The technical scheme adopted by the invention for solving the technical problems is as follows:
an integrated ultrahigh-pressure hydrogen production system of methanol steam and hydrogen mixed gas comprises a three-phase heat exchange device, a reforming device, a hydrogen separation device, a steam trap, a water-cooled heat exchanger, a refrigerator and a carbon dioxide liquefaction device;
the reforming device comprises a reaction cavity, and a heating cavity is arranged outside the reaction cavity; the reaction cavity comprises an upper reaction cavity and a lower reaction cavity, the upper reaction cavity is suitable for reforming methanol steam, the lower reaction cavity is suitable for reforming hydrogen mixed residual gas, and the upper reaction cavity is communicated with the lower reaction cavity;
copper-based filler or zirconium-based filler is filled in the upper reaction cavity, and copper-based filler or zirconium-based filler is filled in the lower reaction cavity; the upper reaction cavity is provided with a first inlet and a first outlet, and the lower reaction cavity is provided with a second inlet;
the first inlet is connected with a methanol steam inlet pipe, the first outlet is connected with an inlet of a hydrogen separation device, the hydrogen separation device is connected with a pure hydrogen gas outlet pipe and a carbon dioxide mixed residual gas outlet pipe, the carbon dioxide mixed residual gas outlet pipe is sequentially connected with a three-phase heat exchange device, a steam trap, a water-cooling heat exchanger and a carbon dioxide liquefaction device, the carbon dioxide liquefaction device is connected with the carbon dioxide outlet pipe and a hydrogen mixed residual gas outlet pipe, the hydrogen mixed residual gas outlet pipe is connected with a second inlet, and an air pump used for increasing the conveying pressure of the hydrogen mixed residual gas in the pipe is arranged on the hydrogen mixed residual gas outlet pipe; the methanol steam inlet pipe and the pure hydrogen outlet pipe are both connected with a three-phase heat exchange device;
the methanol steam inlet pipe is connected with a liquid pump, the pump pressure of the liquid pump is 40-100 MPa, and pure hydrogen in the hydrogen outlet pipe is fed into a hydrogen storage tank under the pump pressure of the liquid pump;
the water-cooling heat exchanger is connected with the water-cooling tower, and the operating temperature of the water-cooling heat exchanger is less than or equal to 30.8 ℃.
Further, the pure hydrogen gas outlet pipe is connected with a hydrogen storage tank, the pure hydrogen gas is pumped into the hydrogen storage tank under the pressure of a liquid pump, the hydrogen storage tank is connected with a hydrogenation machine, and the hydrogen storage tank is connected with the hydrogenation machine.
In another aspect, an ultrahigh pressure hydrogen production method using the above ultrahigh pressure hydrogen production system includes the following steps:
s1, feeding methanol water into a methanol steam pipe inlet pipe by a liquid pump, wherein the pump pressure is 40-100 MPa, heating and vaporizing the methanol water to form methanol steam, feeding the methanol steam into an upper reaction cavity of a reforming device, carrying out reforming reaction on the methanol steam in the upper reaction cavity of the reforming device to generate a mixed gas of hydrogen, carbon dioxide and carbon monoxide, and feeding the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide into a hydrogen separation device;
the gas phase component of the mixed gas of hydrogen, carbon dioxide and carbon monoxide is 65-75% of hydrogen, 20-26% of carbon dioxide and 0.3-3% of carbon monoxide;
s2, separating the mixed gas of hydrogen, carbon dioxide and carbon monoxide by a hydrogen absorption pipe in the hydrogen separation device, outputting the separated pure hydrogen from a pure hydrogen outlet pipe, collecting the pure hydrogen, and sending the pure hydrogen into a hydrogen storage tank under the pump pressure of a liquid pump; the residual carbon dioxide mixed residual gas is output from a carbon dioxide mixed residual gas outlet pipe, the pressure of the carbon dioxide mixed residual gas is controlled by a liquid pump, the temperature of the carbon dioxide mixed residual gas is controlled by a water-cooling heat exchanger, and then the carbon dioxide mixed residual gas is sent into a carbon dioxide separation device for carbon dioxide liquefaction and separation;
the gas phase components of the carbon dioxide mixed residual gas comprise 25-45% of hydrogen, 55-75% of carbon dioxide, 0-3% of water and 0.3-3% of carbon monoxide;
the control pressure of the liquid pump is 40-100 MPa, and the control temperature of the water-cooling heat exchanger is less than or equal to 30.8 ℃;
s3, preparing the carbon dioxide mixed residual gas into liquid carbon dioxide and hydrogen mixed residual gas in a carbon dioxide separator, and outputting and collecting the liquid carbon dioxide;
the components of the hydrogen mixed residual gas comprise 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide;
s4, feeding the hydrogen mixed residual gas into a lower reaction cavity of a reforming device, preparing reforming mixed gas by water distribution, and distributing water according to the content of carbon monoxide, wherein the water distribution ratio (carbon monoxide: water) is 1: 1-20;
water is distributed in the lower reaction chamber to reform the fed hydrogen mixed residual gas into reformed mixed gas, and the gas phase components of the reformed mixed gas comprise 62-77% of hydrogen, 22-27% of carbon dioxide and 0.5-1.5% of carbon monoxide;
so that the proportion of hydrogen, carbon dioxide and carbon monoxide in the reforming mixed gas is close to the proportion of hydrogen, carbon dioxide and carbon monoxide in the mixed gas of hydrogen, carbon dioxide and carbon monoxide;
and S5, enabling the reformed mixed gas to enter the upper reaction cavity to be mixed with the mixed gas of hydrogen, carbon dioxide and carbon monoxide, and after the reformed mixed gas and the mixed gas of hydrogen, carbon dioxide and carbon monoxide are mixed in the upper reaction cavity, sending the mixed gas into the hydrogen separation device together to perform hydrogen separation operation again.
Further, the pure hydrogen of output and carbon dioxide mixed residual gas are all exported after three-phase heat transfer device heat transfer cooling, methanol-water is vaporized into methanol-water vapour through three-phase heat transfer device heat transfer.
Further, the methanol water is replaced by natural gas.
The invention has the beneficial effects that:
the ultrahigh pressure hydrogen production system adopts methanol water as a raw material, the operating pressure of the hydrogen production system is controlled by a liquid pump, hydrogen production is performed under the ultrahigh pressure (40-100 MPa) environment, the operating temperature of carbon dioxide mixed residual gas entering a carbon dioxide separator is controlled by a water-cooling heat exchanger and a water-cooling tower, the temperature is controlled to be less than or equal to 30.8 ℃, and the temperature control of the water-cooling heat exchanger and the water-cooling tower has the advantages of low cost and stable and reliable operation.
The invention has high hydrogen production efficiency, realizes the circular purification of the gas in the system, and can achieve the theoretical yield of 100 percent and the hydrogen yield of more than or equal to 95 percent.
The working method of the methanol-water ultrahigh-pressure hydrogen production system is characterized in that the pressure of methanol water pumped by the liquid pump is controlled at the source of the hydrogen production system to be ultrahigh-pressure (40-100 MPa), the whole hydrogen production system can operate in the ultrahigh-pressure range, the whole hydrogen production system does not need to be provided with equipment such as an air compressor or a compressor for additionally increasing the working pressure of the system, the working pressure of the whole hydrogen production system can be controlled by one liquid pump at the inlet, and the separated pure hydrogen gas, the methanol water and the hydrogen can be directly fed into the system under the ultrahigh-pressure (40-100 MPa) environment,
The pure hydrogen conveying pressure output from the output pipe can also be provided by a liquid pump, so that the inconvenience that a compressor is required to be arranged on the pure hydrogen output pipe to collect the pure hydrogen in the past is eliminated.
According to the ultrahigh-pressure hydrogen production system, the equipment for reforming the methanol steam and the equipment for reforming the hydrogen mixed residual gas in the traditional hydrogen production system are made into one equipment, so that the reforming of the methanol steam and the reforming of the hydrogen mixed residual gas can be carried out in a reaction cavity with the same temperature, the hydrogen production efficiency of the hydrogen production system is improved, the structure of the whole hydrogen production system is optimized and simplified, and the hydrogen production system can be made into small-sized hydrogen production equipment.
The method comprises the steps of recovering carbon dioxide mixed residual gas generated in a hydrogen production system, controlling the pressure and temperature of liquid carbon dioxide separated from the carbon dioxide mixed residual gas through a liquid pump and a water-cooling heat exchanger, separating the carbon dioxide mixed residual gas into hydrogen mixed residual gas and liquid carbon dioxide through a carbon dioxide liquefying device, storing the liquid carbon dioxide, and controlling gas-phase components in the hydrogen mixed residual gas through controlling the pressure and the temperature when the carbon dioxide liquefying device separates, so that the molar ratio of the carbon dioxide in the hydrogen mixed residual gas is lower than 26%, and the hydrogen mixed residual gas is prepared for a subsequent reformed mixed gas; and finally, reforming the hydrogen mixed residual gas through water gas water distribution, reducing carbon monoxide in the hydrogen mixed residual gas from 3-9% originally to 0.5-1.5%, and reforming the gas phase components of the mixed gas: 62-77% of hydrogen, 22-27% of carbon dioxide and 0.5-1.5% of carbon monoxide; the gas phase component of the reformed mixed gas is close to the mixed gas component of the hydrogen, the carbon dioxide and the carbon monoxide prepared by the reformer, the reformed mixed gas and the mixed gas can be mixed and then enter the membrane separation and purification device for hydrogen purification and separation to prepare hydrogen, the gas in the system is circularly purified, the theoretical yield can reach 100 percent, and the hydrogen yield is more than or equal to 95 percent.
Meanwhile, the hydrogen station system for preparing hydrogen by using methanol directly consumes customers, saves freight compared with factory hydrogen in selling price, recovers the hydrogen in the carbon dioxide residual gas, can realize the yield of 100 percent theoretically, is actually more than 90 to 99 percent, and simultaneously recovers CO2Theoretical yield 100 percent and the actual yield is 90 to 99 percent. The process is combined with a hydrogenation station, so that high yield of hydrogen can be realized, and more CO can be recovered2And economic benefit is obtained, safety (high-pressure hydrogen storage is reduced), economy (methanol transportation cost is much lower than that of hydrogen) and CO recovery are really realized2Zero emission is realized, and ecological benefits are obtained.
On the one hand, hydrogen production is harmless and zero-state emission; on the other hand, the carbon dioxide emission reduction is made into methanol, greenhouse gas is changed into useful methanol liquid fuel, the methanol liquid fuel is taken as a hydrogenation station, the solar fuel has rich sources, light, wind, water and nuclear energy are all available, the carbon dioxide hydrogenation is used for preparing the methanol, and the methanol can be transported, stored and transported. The problems of manufacture, storage, transportation, installation and the like are solved in the whole view,
firstly, the liquid sunlight hydrogen station solves the safety problem of the ultrahigh pressure hydrogen station; secondly, the problems of storage, transportation and safety of hydrogen are solved; thirdly, hydrogen can be used as renewable energy to realize the aim of cleaning the whole process; fourthly, the liquid sunlight hydrogenation station can recover carbon dioxide, so that carbon dioxide emission reduction is realized, no further carbon dioxide is generated, and the carbon dioxide is always circulated therein; fifthly, the liquid sunlight hydrogenation station technology can be expanded to other chemical synthesis fields and can also be used for chemical hydrogenation; sixth, the system can be shared with a gas station and a methanol adding station. The system is particularly suitable for community distributed thermoelectric combined energy supply and the existing gas stations.
Drawings
The invention is further described below with reference to the accompanying drawings.
FIG. 1 is a schematic diagram of an ultra-high pressure hydrogen production system of the present invention;
FIG. 2 is a schematic view of a methanol steam and hydrogen mixed gas integrated reforming apparatus;
the device comprises a liquid pump 1, a three-phase heat exchange device 2, a reforming device 3, a heating cavity 31, an upper reaction cavity, a lower reaction cavity 32, a heating cavity 33, a hydrogen separation device 4, a water-cooling heat exchanger 5, a carbon dioxide liquefaction device 6, a steam trap 7, a steam trap 8 and an air pump.
Detailed Description
The invention will now be further described with reference to specific examples. These drawings are simplified schematic diagrams only illustrating the basic structure of the present invention in a schematic manner, and thus show only the constitution related to the present invention.
Example one
As shown in fig. 1 and fig. 2, a methanol steam and hydrogen mixed gas integrated ultrahigh pressure hydrogen production system comprises a three-phase heat exchange device 2, a reforming device 3, a steam trap 7, a hydrogen separation device 4, a water-cooled heat exchanger 5, a refrigerator and a carbon dioxide liquefaction device 6.
The reforming device 3 comprises a reaction cavity, and a heating cavity 33 is arranged outside the reaction cavity; the reaction cavity comprises an upper reaction cavity 31 suitable for reforming reaction of methanol steam and a lower reaction cavity 32 suitable for reforming hydrogen mixed residual gas, and the upper reaction cavity 31 is communicated with the lower reaction cavity 32;
the upper reaction chamber 31 is filled with copper-based filler or zirconium-based filler, the lower reaction chamber 32 is filled with copper-based filler or zirconium-based filler, the upper reaction chamber 31 is provided with a first inlet and a first outlet, and the lower reaction chamber 32 is provided with a second inlet;
the first inlet is connected with a methanol steam inlet pipe, the first outlet is connected with an inlet of a hydrogen separation device 4, the hydrogen separation device 4 is connected with a pure hydrogen gas outlet pipe and a carbon dioxide mixed residual gas outlet pipe, the carbon dioxide mixed residual gas outlet pipe is sequentially connected with a three-phase heat exchange device 2, a steam trap 7, a water-cooling heat exchanger 5 and a carbon dioxide liquefaction device 6, the carbon dioxide liquefaction device 6 is connected with the carbon dioxide outlet pipe and a hydrogen mixed residual gas outlet pipe, the hydrogen mixed residual gas outlet pipe is connected with the second inlet, and an air pump 8 for increasing the conveying pressure of the hydrogen mixed residual gas in the pipe is arranged on the hydrogen mixed residual gas outlet pipe; the methanol steam inlet pipe and the pure hydrogen outlet pipe are both connected with the three-phase heat exchange device 2;
the steam trap 7 is provided to reduce moisture in the carbon dioxide mixed residual gas and prevent excessive moisture from entering the carbon dioxide liquefaction device 6.
The methanol steam inlet pipe is connected with a liquid pump 1, the pump pressure of the liquid pump 1 is 40-100 MPa, and pure hydrogen in the hydrogen outlet pipe is fed into a hydrogen storage tank under the pump pressure of the liquid pump; the water-cooling heat exchanger 5 is connected with a water-cooling tower, and the operating temperature of the water-cooling heat exchanger 5 is less than or equal to 30.8 ℃.
The pure hydrogen gas outlet pipe is connected with a hydrogen storage tank, the pure hydrogen gas is pumped into the hydrogen storage tank under the pressure of a liquid pump, the hydrogen storage tank is connected with a hydrogenation machine, and the hydrogen storage tank is connected with the hydrogenation machine. The hydrogen production system realizes on-site hydrogen production, the prepared hydrogen is directly stored in the hydrogen storage tank, and the prepared pure hydrogen is directly added into the hydrogen vehicle through the hydrogenation machine.
During operation, methanol water is conveyed by the liquid pump 1 and vaporized into methanol steam by the three-phase heat exchange device 2, the working pressure of the liquid pump 1 is 40-100 MPa, the methanol steam enters the upper reaction cavity 31 of the reforming device 3, and the methanol steam is subjected to catalytic reaction in the reformer, so that the multi-component and multi-reaction gas-solid catalytic reaction system is formed;
the reaction equation is: CH (CH)3OH→CO+2H2(ii) a (reversible reaction)
H2O+CO→CO2+H2(ii) a (reversible reaction);
CH3OH+H2O→CO2+3H2(ii) a (reversible reaction);
2CH3OH→CH3OCH3+H2o; (side reaction);
CO+3H2→CH4+H2o; (side reaction);
the reforming reaction generates a mixed gas of hydrogen, carbon dioxide and carbon monoxide. The mixed gas of hydrogen, carbon dioxide and carbon monoxide enters a hydrogen separation device 4 to carry out hydrogen separation operation, a hydrogen absorption pipe in the hydrogen separation device 4 carries out hydrogen absorption separation on the mixed gas of hydrogen, carbon dioxide and carbon monoxide, and the separated pure hydrogen is output from a pure hydrogen outlet pipe; the separated carbon dioxide mixed residual gas is output from a carbon dioxide mixed residual gas outlet pipe, the pressure of the carbon dioxide mixed residual gas is controlled by a hydraulic pump, the temperature is controlled by a water-cooled heat exchanger 5, so that the carbon dioxide mixed residual gas and the carbon dioxide separation device carry out liquefaction separation, separated liquid carbon dioxide is collected, separated hydrogen mixed residual gas is sent into the lower reaction cavity 32 of the reforming device 3, the hydrogen mixed residual gas is changed into reformed mixed gas after water gas reforming in the lower reaction cavity 32, the proportion of gas phase components of the reformed mixed gas and mixed gas components of hydrogen, carbon dioxide and carbon monoxide generated by reforming reaction is approximate, the reformed mixed gas in the lower reaction cavity 32 directly enters the upper reaction cavity 31, and the mixed gas is mixed with the mixed gas of hydrogen, carbon dioxide and carbon monoxide and enters the hydrogen separation device 4 again for circular hydrogen absorption separation, so that the hydrogen yield of the whole ultrahigh-pressure hydrogen production system is improved.
According to the ultrahigh-pressure hydrogen production system, the equipment for reforming the methanol steam and the equipment for reforming the hydrogen mixed residual gas in the traditional hydrogen production system are made into one equipment, so that the reforming of the methanol steam and the reforming of the hydrogen mixed residual gas can be carried out in a reaction cavity with the same temperature, the hydrogen production efficiency of the hydrogen production system is improved, the structure of the whole hydrogen production system is optimized and simplified, and the hydrogen production system can be made into small-sized hydrogen production equipment.
In the ultrahigh-pressure hydrogen production system, an ultrahigh-pressure reforming reaction environment is provided by the liquid pump 1, the pressure provided by the liquid pump 1 is 40-100 MPa, so that when the whole hydrogen production system is used for treating the carbon dioxide mixed residual gas, only the water-cooling heat exchanger 5 is needed to control the temperature (less than or equal to 30.8 ℃) of the carbon dioxide mixed residual gas in the carbon dioxide liquefying device 6, the pressure of the carbon dioxide mixed residual gas in the carbon dioxide liquefying device 6 is directly controlled by the liquid pump 1 from the source, the operating temperature of the carbon dioxide mixed residual gas entering the carbon dioxide separator is controlled by the water-cooling heat exchanger 5 and the water-cooling tower, the temperature control of the water-cooling heat exchanger 5 and the water-cooling tower is controlled to be less than or equal to 30.8 ℃, and the ultrahigh-pressure reforming reaction system has the advantages of low cost and stable and reliable operation, and is suitable for being.
Example two
In another aspect, a method for producing hydrogen by using the above system for producing hydrogen by using ultra-high pressure comprises the following steps:
s1, the liquid pump 1 sends methanol water into a methanol steam pipe inlet pipe, the pump pressure is 40-100 MPa, the methanol water is heated and vaporized into methanol steam which enters a reaction cavity 31 on a reforming device 3, the methanol steam carries out reforming reaction in the reaction cavity 31 on the reforming device 3 to generate mixed gas of hydrogen, carbon dioxide and carbon monoxide, and then the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide is sent into a hydrogen separation device 4;
the methanol vapor carries out catalytic reaction at corresponding temperature and catalyst filler, which is a multi-component and multi-reaction gas-solid catalytic reaction system;
the reaction equation is: CH (CH)3OH→CO+2H2(ii) a (reversible reaction)
H2O+CO→CO2+H2(ii) a (reversible reaction)
CH3OH+H2O→CO2+3H2(ii) a (reversible reaction)
2CH3OH→CH3OCH3+H2O; (side reaction)
CO+3H2→CH4+H2O; (side reaction);
the gas phase component of the mixed gas of hydrogen, carbon dioxide and carbon monoxide is 65-75% of hydrogen, 20-26% of carbon dioxide and 0.3-3% of carbon monoxide;
s2, separating the mixed gas of hydrogen, carbon dioxide and carbon monoxide by a hydrogen absorption pipe in the hydrogen separation device 4, outputting the separated pure hydrogen from a pure hydrogen outlet pipe to be collected, sending the pure hydrogen into a hydrogen storage tank under the pump pressure of a liquid pump, and sending the pure hydrogen into the hydrogen storage tank under the pump pressure of the liquid pump; the residual carbon dioxide mixed residual gas is output from a carbon dioxide mixed residual gas outlet pipe, the pressure of the carbon dioxide mixed residual gas is controlled by a liquid pump 1, the temperature of the carbon dioxide mixed residual gas is controlled by a water-cooled heat exchanger 5, and then the carbon dioxide mixed residual gas is sent into a carbon dioxide separation device for carbon dioxide liquefaction and separation;
the gas phase components of the carbon dioxide mixed residual gas comprise 25-45% of hydrogen, 55-75% of carbon dioxide, 0-3% of water and 0.3-3% of carbon monoxide;
the pressure controlled by the liquid pump 1 is 40-100 MPa, and the temperature controlled by the water-cooled heat exchanger 5 is less than or equal to 30.8 ℃;
s3, preparing the carbon dioxide mixed residual gas into liquid carbon dioxide and hydrogen mixed residual gas in a carbon dioxide separator, and outputting and collecting the liquid carbon dioxide;
the components of the hydrogen mixed residual gas comprise 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide;
controlling the molar ratio of carbon dioxide in the gaseous phase component of the hydrogen mixed residual gas to be 20-26%, wherein the working pressure of a carbon dioxide liquefying device is 40-100 MPa, and the temperature is less than or equal to 30.8 ℃;
s4, feeding the hydrogen mixed residual gas into the lower reaction cavity 32 of the reforming device 3, preparing reforming mixed gas by water distribution, and distributing water according to the content of carbon monoxide, wherein the water distribution ratio (carbon monoxide: water) is 1: 1-20;
the water gas reforming reaction formula is as follows: CO + H2O→CO2+H2；
Water is distributed in the lower reaction cavity 32 to reform the fed hydrogen mixed residual gas into reformed mixed gas, and the gas phase components of the reformed mixed gas comprise 62-77% of hydrogen, 22-27% of carbon dioxide and 0.5-1.5% of carbon monoxide;
so that the proportion of hydrogen, carbon dioxide and carbon monoxide in the reforming mixed gas is close to the proportion of hydrogen, carbon dioxide and carbon monoxide in the mixed gas of hydrogen, carbon dioxide and carbon monoxide;
and S5, the reforming mixed gas enters the upper reaction cavity 31 to be mixed with the mixed gas of hydrogen, carbon dioxide and carbon monoxide, and the reforming mixed gas and the mixed gas of hydrogen, carbon dioxide and carbon monoxide are mixed in the upper reaction cavity 31 and then are sent into the hydrogen separation device 4 together to perform hydrogen separation again.
Specifically, the mixed residual gas of pure hydrogen and carbon dioxide of output all exports after 2 heat transfer cooling of three-phase heat transfer device, the methanol-water vaporizes into methanol-water vapour through 2 heat transfer of three-phase heat transfer device.
In this embodiment, the methanol-water may be replaced by natural gas, and hydrogen is produced from natural gas to obtain a mixed gas of hydrogen, carbon dioxide and carbon monoxide.
The ultrahigh pressure hydrogen production method of the invention relies on the methanol steam and hydrogen mixer integrated ultrahigh pressure hydrogen production system in the first embodiment, methanol water is used as hydrogen production raw material, the liquid pump 1 provides ultrahigh pressure (40-100 MPa) at the source to pump the methanol water into the upper reaction chamber 31 of the reforming device 3, and the mixed gas of hydrogen, carbon dioxide and carbon monoxide is generated by reaction, then the mixed gas of hydrogen, carbon dioxide and carbon monoxide is sent into a hydrogen separation cavity of a hydrogen separation device 4, a hydrogen absorption pipe in the hydrogen separation cavity reacts to absorb hydrogen, the acquired pure hydrogen can be directly output and acquired, and under the ultrahigh pressure (40-100 MPa) environment, the pure hydrogen conveying pressure of the separated pure hydrogen and the pure hydrogen output from the output pipe can be provided by the liquid pump, so that the inconvenience that a compressor needs to be arranged on the pure hydrogen output pipe to collect the pure hydrogen in the prior art is eliminated, and the hydrogen production efficiency is greatly improved.
For the transportation of the generated carbon dioxide mixed residual gas, the pressure and the temperature of the carbon dioxide mixed residual gas in a carbon dioxide separation device are controlled through a liquid preparation pump 1 and a water-cooled heat exchanger 5, so that the carbon dioxide in the carbon dioxide mixed residual gas is liquefied and separated, the components of the separated hydrogen mixed residual gas are controlled, the molar ratio of the carbon dioxide in the hydrogen mixed residual gas is lower than 26 percent, and the hydrogen mixed residual gas is prepared for the subsequent reforming mixed gas; the mixed residual gas of hydrogen is sent into the lower reaction chamber 32 of the reforming device 3 again, and the lower reaction chamber 32 of the reforming device 3 is the same with the operation temperature of the upper reaction chamber 31, and through water gas water distribution reforming, the reformed mixed gas is generated, carbon monoxide in the mixed residual gas of hydrogen is reduced to 0.5-1.5% from 3-9% originally, and the gas phase component of the reformed mixed gas is: 62-77% of hydrogen, 22-27% of carbon dioxide and 0.5-1.5% of carbon monoxide; the gas phase component of the reformed mixed gas is close to the mixed gas component of hydrogen, carbon dioxide and carbon monoxide prepared by the reformer, the reformed mixed gas enters the upper reaction chamber 31, is mixed with the mixed gas of hydrogen, carbon dioxide and carbon monoxide, and enters the hydrogen separation device 4 together again for circular hydrogen absorption separation, so that the gas in the system is circularly purified, the theoretical yield can reach 100%, and the yield of hydrogen is more than or equal to 95%.
In light of the foregoing description of the preferred embodiment of the present invention, many modifications and variations will be apparent to those skilled in the art without departing from the spirit and scope of the invention. The technical scope of the present invention is not limited to the content of the specification, and must be determined according to the claims.
Claims (5)
1. An integrated ultrahigh pressure hydrogen production system of methanol steam and hydrogen mixed gas is characterized by comprising a three-phase heat exchange device, a reforming device, a hydrogen separation device, a steam trap, a water-cooled heat exchanger, a refrigerator and a carbon dioxide liquefaction device;
the reforming device comprises a reaction cavity, and a heating cavity is arranged outside the reaction cavity; the reaction cavity comprises an upper reaction cavity and a lower reaction cavity, the upper reaction cavity is suitable for reforming methanol steam, the lower reaction cavity is suitable for reforming hydrogen mixed residual gas, and the upper reaction cavity is communicated with the lower reaction cavity;
copper-based filler or zirconium-based filler is filled in the upper reaction cavity, and copper-based filler or zirconium-based filler is filled in the lower reaction cavity; the upper reaction cavity is provided with a first inlet and a first outlet, and the lower reaction cavity is provided with a second inlet;
the first inlet is connected with a methanol steam inlet pipe, the first outlet is connected with an inlet of a hydrogen separation device, the hydrogen separation device is connected with a pure hydrogen gas outlet pipe and a carbon dioxide mixed residual gas outlet pipe, the carbon dioxide mixed residual gas outlet pipe is sequentially connected with a three-phase heat exchange device, a steam trap, a water-cooling heat exchanger and a carbon dioxide liquefaction device, the carbon dioxide liquefaction device is connected with the carbon dioxide outlet pipe and a hydrogen mixed residual gas outlet pipe, the hydrogen mixed residual gas outlet pipe is connected with a second inlet, and an air pump used for increasing the conveying pressure of the hydrogen mixed residual gas in the pipe is arranged on the hydrogen mixed residual gas outlet pipe; (ii) a The methanol steam inlet pipe and the pure hydrogen outlet pipe are both connected with a three-phase heat exchange device;
the methanol steam inlet pipe is connected with a liquid pump, the pump pressure of the liquid pump is 40-100 Mpa, and pure hydrogen in the hydrogen outlet pipe is sent into a hydrogen storage tank under the pump pressure of the liquid pump;
the water-cooling heat exchanger is connected with the water-cooling tower, and the operating temperature of the water-cooling heat exchanger is less than or equal to 30.8 ℃.
2. The system of claim 1, wherein the pure hydrogen gas outlet pipe is connected with a hydrogen storage tank, the pure hydrogen gas is pumped into the hydrogen storage tank under the pressure of a liquid pump, the hydrogen storage tank is connected with a hydrogenation machine, and the hydrogen storage tank is connected with the hydrogenation machine.
3. An ultrahigh pressure hydrogen production method is characterized in that the ultrahigh pressure hydrogen production system of claims 1-2 is adopted, and comprises the following steps:
s1, feeding methanol water into a methanol steam pipe inlet pipe by a liquid pump, wherein the pump pressure is 40-100 MPa, heating and vaporizing the methanol water to form methanol steam, feeding the methanol steam into an upper reaction cavity of a reforming device, carrying out reforming reaction on the methanol steam in the upper reaction cavity of the reforming device to generate a mixed gas of hydrogen, carbon dioxide and carbon monoxide, and feeding the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide into a hydrogen separation device;
the gas phase component of the mixed gas of hydrogen, carbon dioxide and carbon monoxide is 65-75% of hydrogen, 20-26% of carbon dioxide and 0.3-3% of carbon monoxide;
s2, separating the mixed gas of hydrogen, carbon dioxide and carbon monoxide by a hydrogen absorption pipe in the hydrogen separation device, outputting the separated pure hydrogen from a pure hydrogen outlet pipe, collecting the pure hydrogen, and sending the pure hydrogen into a hydrogen storage tank under the pump pressure of a liquid pump; the residual carbon dioxide mixed residual gas is output from a carbon dioxide mixed residual gas outlet pipe, the pressure of the carbon dioxide mixed residual gas is controlled by a liquid pump, the temperature of the carbon dioxide mixed residual gas is controlled by a water-cooling heat exchanger, and then the carbon dioxide mixed residual gas is sent into a carbon dioxide separation device for carbon dioxide liquefaction and separation;
the gas phase components of the carbon dioxide mixed residual gas comprise 25-45% of hydrogen, 55-75% of carbon dioxide, 0-3% of water and 0.3-3% of carbon monoxide;
the control pressure of the liquid pump is 40-100 MPa, and the control temperature of the water-cooling heat exchanger is less than or equal to 30.8 ℃;
s3, preparing the carbon dioxide mixed residual gas into liquid carbon dioxide and hydrogen mixed residual gas in a carbon dioxide separator, and outputting and collecting the liquid carbon dioxide;
the components of the hydrogen mixed residual gas comprise 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide;
s4, feeding the hydrogen mixed residual gas into a lower reaction cavity of a reforming device, preparing reforming mixed gas by water distribution, and distributing water according to the content of carbon monoxide, wherein the water distribution ratio (carbon monoxide: water) is 1: 1-20;
water is distributed in the lower reaction chamber to reform the fed hydrogen mixed residual gas into reformed mixed gas, and the gas phase components of the reformed mixed gas comprise 62-77% of hydrogen, 22-27% of carbon dioxide and 0.5-1.5% of carbon monoxide;
so that the proportion of hydrogen, carbon dioxide and carbon monoxide in the reforming mixed gas is close to the proportion of hydrogen, carbon dioxide and carbon monoxide in the mixed gas of hydrogen, carbon dioxide and carbon monoxide;
and S5, enabling the reformed mixed gas to enter the upper reaction cavity to be mixed with the mixed gas of hydrogen, carbon dioxide and carbon monoxide, and after the reformed mixed gas and the mixed gas of hydrogen, carbon dioxide and carbon monoxide are mixed in the upper reaction cavity, sending the mixed gas into the hydrogen separation device together to perform hydrogen separation operation again.
4. The ultrahigh pressure hydrogen production method according to claim 3, wherein the output pure hydrogen and carbon dioxide mixed residual gas are output after being subjected to heat exchange and temperature reduction by a three-phase heat exchange device, and the methanol water is subjected to heat exchange and vaporization by the three-phase heat exchange device to form methanol steam.
5. The ultrahigh pressure hydrogen production process according to claim 3, wherein the methanol-water is replaced with natural gas.
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