CN110790231A - 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 liquefaction device; the carbon dioxide mixed residual gas conveying pipe is connected with a carbon dioxide liquefying device. The separation method comprises the steps of 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, sending the carbon dioxide mixed residual gas into a carbon dioxide liquefying device; the pressure applied to the mixed gas of the 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 hydrogen mixed residual gas comprises 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 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.
At present, the system for producing hydrogen by methanol water is developed by the hospital, and the principle of the hydrogen production system is as follows: heating methanol water into methanol steam, preparing the methanol steam into mixed gas of hydrogen, carbon dioxide and carbon monoxide through a reformer, and separating the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide into mixed residual gas of pure hydrogen and carbon dioxide through a membrane separation and purification device; pure hydrogen is canned and collected, and the carbon dioxide mixed residual gas is mainly directly discharged in the current stage of treating the other part of the carbon dioxide mixed residual gas, and is not recycled, so that the waste is serious; through careful analysis, the part of the carbon dioxide mixed residual gas can be recycled, 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 hydrogen, carbon dioxide and 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, in the first step, the carbon dioxide mixed residual gas is firstly processed by a carbon dioxide liquefying device to separate pure carbon dioxide and hydrogen mixed residual gas, at the moment, the volume ratio of the carbon dioxide in the hydrogen mixed residual gas is adjusted to 20-26% from 55-75%, in the second step, the hydrogen mixed residual gas is processed, the volume ratio of the 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 and purification device again to perform circulation operation due to the fact that the component ratio of the reformed mixed gas is close to the gas phase component ratio of the mixed gas of the hydrogen, the carbon dioxide and the carbon monoxide, so that the hydrogen production yield of the whole system is improved.
Therefore, how to carry out first step, how to carry out reaction treatment to carbon dioxide mixture residual gas promptly in this patent application, in the component of the hydrogen mixture residual gas that makes carbon dioxide mixture residual gas separate, the volume ratio of carbon dioxide can be controlled at 20 ~ 26%, makes it satisfy in the reformed gas mixture to the requirement of carbon dioxide volume ratio.
Disclosure of Invention
The technical problem to be solved by the invention is as follows: the system and the method overcome the defects of the prior art, and the carbon dioxide mixed residual gas separation system and the method thereof are provided, so that the problem that the content of carbon dioxide in the carbon dioxide mixed residual gas generated by a methanol water hydrogen production system is adjusted to 20-26% from 55-75% to meet the requirement of the reformed mixed gas on the volume ratio of the carbon dioxide is solved.
The technical scheme adopted by the invention 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 liquefaction 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, set gradually first heat exchanger and second heat exchanger on the carbon dioxide mixed residual gas conveyer pipe, first heat exchanger and second heat exchanger carry out the heat transfer with methanol-water, reduce the temperature of the carbon dioxide mixed residual gas that carries in the carbon dioxide mixed residual gas conveyer pipe.
Further, an air compressor 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 is arranged at the downstream of the second heat exchanger;
and a steam trap for reducing the moisture 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, feeding the mixed gas of hydrogen, carbon dioxide and carbon monoxide into a membrane separation hydrogen production device at a controlled temperature, wherein the membrane separation hydrogen production device separates the fed mixed gas of 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;
the pure hydrogen is collected into a hydrogen storage tank of a hydrogenation station;
the gas phase components of the mixed gas of hydrogen, carbon dioxide and carbon monoxide comprise 65-75% of hydrogen, 20-26% of carbon dioxide and 0.3-3% of 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, sending 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 the carbon dioxide is 5-30 Mpa, and the operating 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 hydrogen mixed residual gas comprises 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide.
Further, the pressure and temperature of the carbon dioxide liquefaction plant during operation are selected as follows:
| scheme(s) | 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 used for producing hydrogen by palladium membrane separation or niobium membrane separation.
Further, the mixed gas of hydrogen, carbon dioxide and carbon monoxide is produced by methanol-water reforming or by natural gas reforming.
The invention has the beneficial effects that:
the carbon dioxide mixed residual gas is separated into pure carbon dioxide and hydrogen mixed residual gas by controlling the pressure and the temperature of the carbon dioxide mixed residual gas in a carbon dioxide liquefying device, and the volume ratio of the carbon dioxide in the components of the separated hydrogen mixed residual gas can be controlled to be 20-26%, so that the requirement of the reformed mixed gas on the volume ratio of the carbon dioxide is met.
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 high-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 a carbon dioxide mixed residual gas separation system for a low pressure hydrogen production system;
the system comprises a membrane separation hydrogen production device 1, a carbon dioxide liquefaction device 2, a first heat exchanger 31, a second heat exchanger 32, an air compressor 4, a first temperature controller 51, a second 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 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, 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 liquefaction 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.
Set gradually first heat exchanger 31 and second heat exchanger 32 on the carbon dioxide mixes the residual gas conveyer pipe, first heat exchanger 31 and second heat exchanger 32 carry out the heat transfer with methanol-water, reduce the temperature of the carbon dioxide that carries mixes the residual gas in the carbon dioxide mixes the residual gas conveyer pipe.
The working temperature of the membrane separation hydrogen production device 1 is 380-420 ℃, the temperature of pure hydrogen separated is 380-420 ℃, and the temperature of carbon dioxide mixed residual gas separated 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;
and a steam trap 6 for reducing the moisture of the carbon dioxide mixed residual gas in the pipe is arranged between the air compressor and the second heat exchanger.
The carbon dioxide mixed residual gas conveying pipe is provided with a first temperature controller 51 and a second temperature controller 52, 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 carbon dioxide mixed residual gas separation method for the low-pressure hydrogen production system comprises the following steps:
s1, heating and evaporating the methanol water to obtain methanol steam, and allowing the methanol steam to enter a reformer for reforming reaction to obtain a mixed gas of hydrogen, carbon dioxide and carbon monoxide; the gas phase components of the mixed gas of hydrogen, carbon dioxide and carbon monoxide comprise 65-75% of hydrogen, 20-26% of carbon dioxide and 0.3-3% of carbon monoxide; the methanol water is conveyed by a conveying pump, the pressure of the conveying pump is 2-5 MPa and 2-5 MPa, and the low-pressure hydrogen production system belongs to the low-pressure hydrogen production system.
Controlling the temperature of the mixed gas of hydrogen, carbon dioxide and carbon monoxide, and feeding the mixed gas into a membrane separation hydrogen production device 1, wherein the membrane separation hydrogen production device 1 separates the fed mixed gas of 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;
the pure hydrogen is collected 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, sending 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 the 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 hydrogen mixed residual gas comprises 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide.
Specifically, the pressure and temperature of the carbon dioxide liquefaction plant 2 during operation are selected as follows:
| scheme(s) | 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 apparatus is a palladium membrane separation hydrogen production apparatus or a niobium membrane separation hydrogen production apparatus.
In this embodiment, the mixed gas of hydrogen, carbon dioxide and carbon monoxide is obtained by methanol-water reforming or natural gas reforming.
In the embodiment, the pressure of the carbon dioxide mixed residual gas output from the membrane separation hydrogen production device 1 is 2-5 MPa, which is low pressure and relatively safe, so that the pressure and the temperature of the carbon dioxide mixed residual gas in the carbon dioxide liquefaction 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%, a reformer is required to be carried out subsequently on the hydrogen mixed residual gas, carbon monoxide in the hydrogen mixed residual gas is further removed, the finally prepared reformed mixed gas has components close to the mixed gas of hydrogen, carbon dioxide and carbon monoxide, and circulation can be carried out, in the embodiment, the membrane separation hydrogen production device is mainly responsible for controlling the volume ratio of the carbon dioxide in the reformed mixed gas, controlling the content of the active ingredients to be 20-26%; by adopting the separation method of the embodiment, the hydrogen mixed residual gas meeting the requirements can be separated.
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 scope of the claims.
Claims (8)
1. A carbon dioxide mixed residual gas separation system for a low-pressure hydrogen production system is characterized by comprising a membrane separation hydrogen production device and a carbon dioxide liquefaction 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.
2. The carbon dioxide mixed residual gas separation system for the low-pressure hydrogen production system according to claim 1, wherein 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 to reduce the temperature of the carbon dioxide mixed residual gas conveyed in the carbon dioxide mixed residual gas conveying pipe.
3. The carbon dioxide mixed residual gas separation system for the low-pressure hydrogen production system according to claim 2, wherein an air compressor 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 is arranged at the downstream of the second heat exchanger;
and a steam trap for reducing the moisture of the carbon dioxide mixed residual gas in the pipe is arranged between the air compressor and the second heat exchanger.
4. The carbon dioxide mixed residual gas separation system for the low-pressure hydrogen production system according to claim 3, wherein 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.
5. A carbon dioxide mixed residual gas separation method, which is characterized in that the separation system of any one of claims 1 to 4 is adopted, and comprises the following steps:
s1, feeding the mixed gas of hydrogen, carbon dioxide and carbon monoxide into a membrane separation hydrogen production device at a controlled temperature, wherein the membrane separation hydrogen production device separates the fed mixed gas of 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;
the pure hydrogen is collected into a hydrogen storage tank of a hydrogenation station;
the gas phase components of the mixed gas of hydrogen, carbon dioxide and carbon monoxide comprise 65-75% of hydrogen, 20-26% of carbon dioxide and 0.3-3% of 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, sending 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 the carbon dioxide is 5-30 Mpa, and the operating 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 hydrogen mixed residual gas comprises 65-75% of hydrogen, 20-26% of carbon dioxide and 3-9% of carbon monoxide.
6. The carbon dioxide mixed residual gas separation method based on the methanol-water hydrogen production system as claimed in claim 1, wherein the selection of the pressure and the temperature of the carbon dioxide liquefying device during working is as follows:
7. The carbon dioxide mixed residual gas separation method based on the methanol-water hydrogen production system according to claim 1, wherein the membrane separation hydrogen production device is a palladium membrane separation hydrogen production device or a niobium membrane separation hydrogen production device.
8. The method for separating the carbon dioxide mixed residual gas based on the methanol-water hydrogen production system according to claim 1, wherein the mixed gas of hydrogen, carbon dioxide and carbon monoxide is obtained by methanol-water reforming or natural gas reforming.
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