CN110790231B - Carbon dioxide mixed residual gas separation system for low-pressure hydrogen production system and method thereof - Google Patents
Carbon dioxide mixed residual gas separation system for low-pressure hydrogen production system and method thereof Download PDFInfo
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Abstract
The invention relates to a carbon dioxide mixed residual gas separation system for a low-pressure hydrogen production system, which comprises a membrane separation and purification device and a carbon dioxide liquefying device; the carbon dioxide mixed residual gas conveying pipe is connected with the carbon dioxide liquefying device. S1, separating carbon dioxide mixed residual gas by a membrane separation and purification device; 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; s2, delivering the carbon dioxide mixed residual gas into a carbon dioxide liquefying device; the pressure applied to the mixed gas of carbon dioxide is 5-15 Mpa, and the operation temperature is-35-30.8 ℃; the carbon dioxide liquefying device separates the carbon dioxide mixed residual gas into liquid carbon dioxide and hydrogen mixed residual gas; the components of the hydrogen mixed residual gas are 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide.
Description
Technical Field
The invention relates to a carbon dioxide mixed residual gas separation system for a low-pressure hydrogen production system and a method thereof.
Background
The hydrogen energy is used as 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 the 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 traditional automobile can be simplified. Of further interest is the addition of only 4% hydrogen to the gasoline. The fuel can save fuel by 40% when used as fuel of automobile engine, and does not need to improve the gasoline engine. The hydrogen fuel cell serves as a power generation system.
The fuel cell has no pollution to the environment. It is by electrochemical reaction, rather than by combustion (gasoline, diesel) or energy storage (battery) means-most typically conventional back-up power schemes. Combustion releases contaminants such as COx, NOx, SOx gas and dust. As described above, the fuel cell generates only water and heat. If hydrogen is generated by renewable energy sources (photovoltaic panels, wind power generation and the like), the whole cycle is a complete process without harmful substance emission.
The fuel cell operates quietly without noise, which is only about 55dB, corresponding to the level of normal human conversation. This makes the fuel cell suitable for a wider range including indoor installation or where noise is limited outdoors.
The high efficiency, the generating efficiency of the fuel cell can reach more than 50%, which is determined by the conversion property of the fuel cell, directly converts chemical energy into electric energy without intermediate conversion of heat energy and mechanical energy (generator), because the efficiency is reduced once more by one energy conversion.
At present, the main source of hydrogen in a hydrogen energy hydrogenation station is that an energy storage tank is used for transporting the hydrogen back from the outside, and the whole hydrogenation station needs to store a large amount of hydrogen; the research shows that the 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, namely the hydrogen preparation and the hydrogen addition, are safer at present, the hydrogen storage link is easier to generate accidents, and the cost of the hydrogen transportation link is higher, so that the hydrogen transportation link is related to the characteristics of the hydrogen; at present, the problem of explosion of a hydrogenation station and the reason of high hydrogenation cost often occur in news.
At present, the system for producing hydrogen by means of methanol water is developed in our hospital, and the principle of the hydrogen production system is as follows: heating methanol water into methanol vapor, preparing the methanol vapor into mixed gas of hydrogen, carbon dioxide and carbon monoxide by a reformer, and separating the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide into pure hydrogen and carbon dioxide mixed residual gas by a membrane separation and purification device; pure hydrogen is collected by canning, and the other part of the separated carbon dioxide mixed residual gas is mainly discharged directly at the current stage of treating the carbon dioxide mixed residual gas, and is not recycled, so that waste is serious; through careful analysis, the carbon dioxide mixed residual gas can be recovered, and the gas phase components of the carbon dioxide mixed residual gas are as follows: 25-45% of hydrogen, 55-75% of carbon dioxide, 0-3% of water and 0.3-3% of carbon monoxide; in the hydrogen production system, the gas phase components of the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide entering the membrane separation and purification device are 65-75% of hydrogen, 20-26% of carbon dioxide and 0.3-3% of carbon monoxide; therefore, only two steps are needed, firstly, the carbon dioxide mixed residual gas is separated from pure carbon dioxide and hydrogen mixed residual gas through a carbon dioxide liquefying device, at the moment, the volume ratio of carbon dioxide in the hydrogen mixed residual gas is adjusted to 20-26% from 55-75%, secondly, the hydrogen mixed residual gas is operated, the volume ratio of hydrogen is adjusted to 65-75% from 25-45%, the carbon dioxide mixed residual gas can be gradually changed into reformed mixed gas, and the reformed mixed gas can enter the membrane separation purifying device again for circulation operation due to the fact that the component ratio is close to the gas phase component ratio of the mixed gas of hydrogen, carbon dioxide and carbon monoxide, and the hydrogen production yield of the whole system is improved.
Therefore, the method mainly solves the problem of how to perform the first step, namely how to perform reaction treatment on the carbon dioxide mixed residual gas, so that the volume ratio of carbon dioxide in the components of the hydrogen mixed residual gas separated from the carbon dioxide mixed residual gas can be controlled to be 20-26%, and the requirements of the reformed mixed gas on the volume ratio of the carbon dioxide are met.
Disclosure of Invention
The invention aims to solve the technical problems that: the carbon dioxide mixed residual gas separation system and the method thereof for the low-pressure hydrogen production system are provided to solve the problem that the content of carbon dioxide in the carbon dioxide mixed residual gas generated by the methanol-water hydrogen production system is adjusted from 55 to 75 percent to 20 to 26 percent so as to meet the requirement of the reformed mixed gas on the volume ratio of the carbon dioxide.
The technical scheme adopted for solving the technical problems is as follows:
a carbon dioxide mixed residual gas separation system for a low-pressure hydrogen production system comprises a membrane separation hydrogen production device and a carbon dioxide liquefying device;
the membrane separation hydrogen production device is connected with a hydrogen output pipe and a carbon dioxide mixed residual gas conveying pipe;
the carbon dioxide mixed residual gas conveying pipe is connected with the carbon dioxide liquefying device, and the carbon dioxide liquefying device is connected with the pure carbon dioxide output pipe and the hydrogen mixed residual gas conveying pipe.
Further, a first heat exchanger and a second heat exchanger are sequentially arranged on the carbon dioxide mixed residual gas conveying pipe, and the first heat exchanger and the second heat exchanger exchange heat with methanol water, so that the temperature of the carbon dioxide mixed residual gas conveyed in the carbon dioxide mixed residual gas conveying pipe is reduced.
Further, an air compressor for controlling the pressure of the carbon dioxide mixed residual air in the pipeline is arranged on the carbon dioxide mixed residual air conveying pipe, and the air compressor is arranged at the downstream of the second heat exchanger;
and a steam trap for reducing the water content of the carbon dioxide mixed residual gas in the pipe is arranged between the air compressor and the second heat exchanger.
Further, a first temperature controller and a second temperature controller are arranged on the carbon dioxide mixed residual gas conveying pipe, and the air compressor is arranged on the carbon dioxide mixed residual gas conveying pipe between the first temperature controller and the second temperature controller, so that the carbon dioxide mixed residual gas separation method is provided, and comprises the following steps:
s1, sending mixed gas of hydrogen, carbon dioxide and carbon monoxide into a membrane separation hydrogen production device in a temperature-controlled manner, wherein the membrane separation hydrogen production device separates the sent mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide into pure hydrogen and carbon dioxide mixed residual gas; the pressure of the mixed residual gas of the pure hydrogen and the carbon dioxide is 2-5 MPa;
collecting the pure hydrogen into a hydrogen storage tank of a hydrogenation station;
the gas phase components of the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide are 65-75% of the hydrogen, 20-26% of the carbon dioxide and 0.3-3% of the carbon monoxide;
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;
s2, delivering the carbon dioxide mixed residual gas into a carbon dioxide liquefying device;
when the carbon dioxide liquefying device works, the pressure applied to the mixed gas of carbon dioxide is 5-30 Mpa, and the working temperature is-35-30.8 ℃;
the carbon dioxide liquefying device separates the carbon dioxide mixed residual gas into liquid carbon dioxide and hydrogen mixed residual gas;
the liquid carbon dioxide is collected;
the components of the hydrogen mixed residual gas are 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide.
Further, the selection of pressure and temperature of the carbon dioxide liquefying device during operation is shown in the following table:
| scheme for the production of a semiconductor device | Pressure (Mpa) | Temperature (. Degree. C.) |
| Scheme 1 | 5 | -35 |
| Scheme 2 | 7 | -25 |
| Scheme 3 | 10 | -10 |
| Scheme 4 | 15 | 0 |
| Scheme 5 | 20 | 20 |
| Scheme 6 | 25 | 25 |
| Scheme 7 | 30 | 30.8 |
Further, the membrane separation hydrogen production device is palladium membrane separation hydrogen production or niobium membrane separation hydrogen production.
Further, the mixed gas of hydrogen, carbon dioxide and carbon monoxide is prepared by reforming methanol water or natural gas.
The beneficial effects of the invention are as follows:
the carbon dioxide mixed residual gas separation system and the separation method for the low-pressure hydrogen production system are provided, the pressure and the temperature of the carbon dioxide mixed residual gas in a carbon dioxide liquefying device are controlled, the carbon dioxide mixed residual gas is separated into pure carbon dioxide and hydrogen mixed residual gas, and the volume ratio of carbon dioxide in the separated hydrogen mixed residual gas can be controlled to be 20-26%, so that the carbon dioxide mixed residual gas meets the requirement of the reformed mixed gas on the volume ratio of carbon dioxide.
On the one hand, hydrogen production is harmless, and zero-state emission is realized; on the other hand, the emission of carbon dioxide is reduced to be made into methanol, the greenhouse gas is changed into useful methanol liquid fuel, the methanol liquid fuel is taken as a hydrogenation station, the source of solar fuel is very rich, light, wind, water and nuclear energy can be all used, the methanol can be prepared by hydrogenating the carbon dioxide, and the storage and transportation of the methanol are not problems. Solves the problems of manufacturing, storing, transporting, installing and the like in the whole,
firstly, the liquid sunlight hydrogenation station solves the safety problem of the high-pressure hydrogenation station; secondly, the problems of hydrogen storage, transportation and safety are solved; thirdly, hydrogen can be used as a renewable energy source to realize the aim of full-flow cleaning; fourthly, the liquid state sunlight hydrogenation station can recycle carbon dioxide, so that carbon dioxide emission reduction is realized, carbon dioxide is not further generated, and the carbon dioxide circulates at the position all the time; fifth, the liquid sunlight hydrogenation station technology can be extended to other chemical synthesis fields, and can also be used for chemical hydrogenation; sixth, the system can be multi-element co-station with a gas station or a methanol adding station. The system is particularly suitable for energy supply and current gas stations for community distributed combined heat and power.
Drawings
The invention is further described below with reference to the accompanying drawings.
FIG. 1 is a schematic diagram of a carbon dioxide mixed residual gas separation system for a low pressure hydrogen system;
the device comprises a membrane separation hydrogen production device 1, a carbon dioxide liquefying device 2, a first heat exchanger 31, a second heat exchanger 32, a first temperature controller 4, an air compressor 51, a first temperature controller 52, a second temperature controller 6 and a steam trap.
Detailed Description
The invention will now be further described with reference to specific examples. These drawings are simplified schematic views illustrating the basic structure of the present invention by way of illustration only, and thus show only the constitution related to the present invention.
Example 1
As shown in fig. 1, a carbon dioxide mixed residual gas separation system for a low-pressure hydrogen production system comprises a membrane separation hydrogen production device 1 and a carbon dioxide liquefying device 2; the membrane separation hydrogen production device 1 is connected with a hydrogen output pipe and a carbon dioxide mixed residual gas conveying pipe; the carbon dioxide mixed residual gas conveying pipe is connected with the carbon dioxide liquefying device 2, and the carbon dioxide liquefying device 2 is connected with the pure carbon dioxide output pipe and the hydrogen mixed residual gas conveying pipe.
The first heat exchanger 31 and the second heat exchanger 32 are sequentially arranged on the carbon dioxide mixed residual gas conveying pipe, and the first heat exchanger 31 and the second heat exchanger 32 exchange heat with methanol water to reduce the temperature of the carbon dioxide mixed residual gas conveyed in the carbon dioxide mixed residual gas conveying pipe.
The working temperature of the membrane separation hydrogen production device 1 is 380-420 ℃, the temperature of separating out pure hydrogen is 380-420 ℃, and the temperature of the carbon dioxide mixed residual gas is 380-420 ℃; the heat exchange temperature of the second heat exchanger 32 is about 300 ℃, and the heat exchange temperature of the first heat exchanger 31 is about 200 ℃.
An air compressor 4 for controlling the pressure of the carbon dioxide mixed residual gas in the pipeline is arranged on the carbon dioxide mixed residual gas conveying pipe, and the air compressor 4 is arranged at the downstream of the second heat exchanger 32;
a steam trap 6 for reducing the water content of the carbon dioxide mixed residual gas in the pipe is arranged between the air compressor and the second heat exchanger.
The first temperature controller 51 and the second temperature controller 52 are arranged on the carbon dioxide mixed residual gas conveying pipe, and the air compressor 4 is arranged on the carbon dioxide mixed residual gas conveying pipe between the first temperature controller 51 and the second temperature controller 52. The two temperature controllers are used for controlling the temperature of the carbon dioxide mixed residual gas.
The carbon dioxide mixed residual gas separation system for the low-pressure hydrogen production system can stably convey the high-temperature carbon dioxide mixed residual gas output by the membrane separation hydrogen production device 1 into the carbon dioxide liquefying device 2, so that the carbon dioxide mixed residual gas can be separated in the carbon dioxide liquefying device 2.
Example two
The method for separating the carbon dioxide mixed residual gas aiming at the low-pressure hydrogen production system comprises the following steps:
s1, heating and evaporating methanol water to obtain methanol water vapor, and enabling the methanol water vapor to enter a reformer for reforming reaction to obtain mixed gas of hydrogen, carbon dioxide and carbon monoxide; the gas phase components of the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide are 65-75% of the hydrogen, 20-26% of the carbon dioxide and 0.3-3% of the carbon monoxide; the methanol water is conveyed by a conveying pump, the pressure is 2-5 MPa, and belongs to the low pressure category, so that the whole hydrogen production system belongs to a low-pressure hydrogen production system.
The mixed gas of hydrogen, carbon dioxide and carbon monoxide is sent into a membrane separation hydrogen production device 1 in a temperature-controlled manner, and the membrane separation hydrogen production device 1 separates the mixed gas of the sent hydrogen, carbon dioxide and carbon monoxide into pure hydrogen and carbon dioxide mixed residual gas; the pressure of the mixed residual gas of the pure hydrogen and the carbon dioxide is 2-5 MPa;
collecting the pure hydrogen into a hydrogen storage tank of a hydrogenation station;
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;
s2, delivering the carbon dioxide mixed residual gas into a carbon dioxide liquefying device 2;
when the carbon dioxide liquefying device 2 works, the pressure applied to the mixed gas of carbon dioxide is 5-30 Mpa, and the working temperature is-35-30.8 ℃;
the carbon dioxide liquefying device 2 separates the carbon dioxide mixed residual gas into liquid carbon dioxide and hydrogen mixed residual gas;
the liquid carbon dioxide is collected;
the components of the hydrogen mixed residual gas are 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide.
Specifically, the selection of the pressure and the temperature of the carbon dioxide liquefying device 2 during operation is shown in the following table:
| scheme for the production of a semiconductor device | Pressure (MPa) | Temperature (. Degree. C.) |
| Scheme 1 | 5 | -35 |
| Scheme 2 | 7 | -25 |
| Scheme 3 | 10 | -10 |
| Scheme 4 | 15 | 0 |
| Scheme 5 | 20 | 20 |
| Scheme 6 | 25 | 25 |
| Scheme 7 | 30 | 30.8 |
In this embodiment, the membrane separation hydrogen production device is palladium membrane separation hydrogen production or niobium membrane separation hydrogen production.
In this embodiment, the mixed gas of hydrogen, carbon dioxide and carbon monoxide is prepared by reforming methanol-water or natural gas.
In this embodiment, the pressure of the carbon dioxide mixed residual gas output from the membrane separation hydrogen production device 1 is 2-5 MPa, which belongs to low pressure and is relatively safe, so that the pressure and the temperature of the carbon dioxide mixed residual gas in the carbon dioxide liquefying device 2 are controlled by an air compressor, the carbon dioxide mixed residual gas is separated into pure carbon dioxide and hydrogen mixed residual gas, the volume ratio of the carbon dioxide in the separated hydrogen mixed residual gas can be controlled to be 20-26%, the hydrogen mixed residual gas is further subjected to a water gas reformer, and carbon monoxide in the hydrogen mixed residual gas is further removed, so that the finally prepared reformed mixed gas is close to the mixed gas of hydrogen, carbon dioxide and carbon monoxide, and the cyclic hydrogen production can be performed; by adopting the separation method of the embodiment, the hydrogen mixed residual gas meeting the requirements can be separated.
With the above-described preferred embodiments according to the present invention as an illustration, the above-described descriptions can be used by persons skilled in the relevant art to make various changes and modifications without departing from the scope of the technical idea of the present invention. The technical scope of the present invention is not limited to the description, but must be determined according to the scope of claims.
Claims (4)
1. A method for separating carbon dioxide mixed residual gas is characterized by adopting a separation system, wherein the separation system comprises
A membrane separation hydrogen production device and a carbon dioxide liquefying device;
the membrane separation hydrogen production device is connected with a hydrogen output pipe and a carbon dioxide mixed residual gas conveying pipe;
the carbon dioxide mixed residual gas conveying pipe is connected with a carbon dioxide liquefying device, and the carbon dioxide liquefying device is connected with a pure carbon dioxide output pipe and a hydrogen mixed residual gas conveying pipe;
the first heat exchanger and the second heat exchanger are sequentially arranged on the carbon dioxide mixed residual gas conveying pipe and exchange heat with methanol water, so that the temperature of the carbon dioxide mixed residual gas conveyed in the carbon dioxide mixed residual gas conveying pipe is reduced;
the air compressor is used for controlling the pressure of the carbon dioxide mixed residual air in the pipeline and is arranged at the downstream of the second heat exchanger;
a steam trap for reducing the water content of the carbon dioxide mixed residual gas in the pipe is arranged between the air compressor and the second heat exchanger;
the air compressor is arranged on the carbon dioxide mixed residual gas conveying pipe between the first temperature controller and the second temperature controller;
the method comprises the following steps:
s1, sending mixed gas of hydrogen, carbon dioxide and carbon monoxide into a membrane separation hydrogen production device in a temperature-controlled manner, wherein the membrane separation hydrogen production device separates the sent mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide into pure hydrogen and carbon dioxide mixed residual gas; the pressure of the mixed residual gas of the pure hydrogen and the carbon dioxide is 2-5 MPa;
collecting the pure hydrogen into a hydrogen storage tank of a hydrogenation station;
the gas phase components of the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide are 65-75% of the hydrogen, 20-26% of the carbon dioxide and 0.3-3% of the carbon monoxide;
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;
s2, delivering the carbon dioxide mixed residual gas into a carbon dioxide liquefying device;
when the carbon dioxide liquefying device works, the pressure applied to the mixed gas of carbon dioxide is 5-30 Mpa, and the working temperature is-35-30.8 ℃;
the carbon dioxide liquefying device separates the carbon dioxide mixed residual gas into liquid carbon dioxide and hydrogen mixed residual gas;
the liquid carbon dioxide is collected;
the components of the hydrogen mixed residual gas are 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide.
2. The method for separating carbon dioxide mixed residual gas according to claim 1, wherein the pressure and temperature of the carbon dioxide liquefying device during operation are selected as follows:
。
3. The method for separating carbon dioxide mixed residual gas according to claim 1, wherein the membrane separation hydrogen production device is palladium membrane separation hydrogen production or niobium membrane separation hydrogen production.
4. The method for separating carbon dioxide mixed gas as claimed in claim 1, wherein the mixed gas of hydrogen, carbon dioxide and carbon monoxide is produced by reforming methanol water or natural gas.
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