CN101306302A - Hydrogen containing industrial waste gas separation and purification method - Google Patents
Hydrogen containing industrial waste gas separation and purification method Download PDFInfo
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- CN101306302A CN101306302A CNA2008100332868A CN200810033286A CN101306302A CN 101306302 A CN101306302 A CN 101306302A CN A2008100332868 A CNA2008100332868 A CN A2008100332868A CN 200810033286 A CN200810033286 A CN 200810033286A CN 101306302 A CN101306302 A CN 101306302A
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Abstract
The invention relates to a separation and purification method for hydrogen-containing industrial waste gas of the field of environmental protection technology, which comprises the steps as follows: the industrial waste gas is humidified by a gas humidifier and then directly introduced to gas separation cells with a multi-level series connection structure, an external DC power supply provides power energy to the cells in a gas separation cell stack; hydrogen in the industrial waste gas is pumped or separated to a high-pressure cathode from a low-pressure anode, the hydrogen with improved pressure and purity is obtained at the gas outlet of the final cell cathode; the residual waste gas after passing through the gas separation cells is sent to a water-gas separation tank to remove the water and is emitted; the recycled water enters a water storage tank, the water supplement without saline water is simultaneously carried out in the water storage tank, and a water circulating pump is utilized for allowing the recycled water to be introduced into the gas humidifier, thereby forming a water circulation. The separation and purification method of the electrochemical cell technology of the invention utilizes a proton exchange membrane as an electrolyte, utilizes the hydrogen-containing industrial waste gas for power generation, and achieves the purposes of hydrogen recycling and utilization, energy conservation and consumption reduction.
Description
Technical field
What the present invention relates to is a kind of waste gas processing method of environmental technology field, specifically is a kind of electrochemical principle separation and purification hydrogen containing industrial waste gas method utilized.
Background technology
Under the background of energy crisis, some high energy-consuming industries are more and more paid attention to the saving of the energy and utilization.Enlarge the hydrogen gas production resource, develop new process for making hydrogen and improve existing process for making hydrogen and be subjected to common concern.Ammonia factory in the chemical industry speed venting, methanol-fueled exhaust, acetylene carbon black gas, diene tail gas etc. all contain a certain amount of hydrogen.Utilize hydrogen purification device purifying chemical plant waste gas, purification obtains the hydrogen of higher degree, for industrial enterprise provides the hydrogen goods of various purity, serve fields such as semiconductor, integrated circuit, metallurgy, petrochemical industry, chlor-alkali, formaldehyde, float glass, essence and flavoring agent, agricultural production.Therefore, how to separate, purify, utilize the hydrogen in these waste gas to become one of energy-saving and cost-reducing important channel.
Now, the method for recycling hydrogen mainly contains Deep Cooling Method, three kinds of pressure swing adsorption method and embrane methods in the industrial production.Every kind of industry all has the advantage of their uniquenesses, and the principle of utilization also has nothing in common with each other, and adapts to use corresponding occasion.The method that the present invention relates to mainly is to utilize the blowback of fuel cell system configuration electrochemical hydrogen to receive high-purity high pressure hydrogen,, and can be connected with the generating equipment of factory, directly utilize the hydrogen that reclaims to give Factory Electricity Supply by fuel cell, have a extensive future.
Find through literature search prior art, United States Patent (USP) 6,280,865 " Fuel cell systemwith hydrogen purification subsystem " have introduced and have utilized Proton Exchange Membrane Fuel Cells to recycle excessive or unreacted hydrogen in the anode of fuel cell tail gas.Mainly be by constructing an electrochemical pump, the energy that hydrogen utilization additional power source excessive in the anode exhaust gas is provided sees through the recovery supercharging utilization of PEM to this part gas, has reduced the job costs of fuel cell, has improved energy utilization rate.Its weak point is: the related method limitation of this patent is very big, be only limited to purifying and reclaim excessive hydrogen in the anode of fuel cell tail gas, can not carry out the separation and the pressurization of hydrogen to the gas of complicated component, under high pressure conditions, store and use because hydrogen is many, and because small scale, the hydrogen as energy source of saving does not have energy-saving significance significantly with respect to the consumption of external direct current energy.Consider that a large amount of industrial hydrogeneous waste gas does not obtain reasonable use, and the system scale effect, so electrochemistry recover hydrogen range of application is wide more, economic function is outstanding.
Summary of the invention
The objective of the invention is to overcome deficiency of the prior art, a kind of separation be provided and purify the hydrogen containing industrial waste gas method, make its utilize the PEM technical point from, purify, utilize the hydrogen containing industrial waste gas generating, reach energy saving purposes.
The present invention is achieved through the following technical solutions, the present invention includes following steps:
The first step, industrial waste gas (hydrogen-containing gas) is passed through the gas moistener humidification earlier, directly be passed into electrochemistry hydrogen pump battery then, just the gas split cell---the gas split cell is the plural serial stage structure that a plurality of fuel cells form, and provides electric energy to the PEM in the fuel cell pack with outer dc source;
Second step, hydrogen in the mist is extracted into or separates negative electrode to high pressure from the anode of low pressure, according to proton membrane technology principle, by the plural serial stage structure, raising Hydrogen Vapor Pressure and purity that can be progressive, thus the gas outlet of a final GND in the end obtains high-purity, high pressure hydrogen.In general, since PEM to hydrogen ion (H
+) selectivity and uniqueness, the hydrogen purity that purifies, reclaims is greater than more than 99.99%, and by means of the pressurization of hydrogen pump, the Hydrogen Vapor Pressure of recovery can improve more than 50% on the original basis.
The 3rd step by the gas behind the gas split cell, mainly was that those non-hydrogen pneumatolytics divide and battery operated needed steam.At this moment, they are passed into the aqueous vapor knockout drum, remove moisture after, remainder of exhaust gas is discharged.
In the 4th step, the moisture of recovery enters into water storage tank, does not have the salt solution moisturizing simultaneously in water storage tank, utilizes water-circulating pump that it is passed into gas moistener, has formed a water circulation.
The present invention is high-purity, the high pressure hydrogen that produce in the process in second step, can directly feed in the hydrogen gas tank they are stored, and offers fuel cell generation as high-purity hydrogen, to give Factory Electricity Supply, perhaps uses as industrial chemicals.
Described gas split cell, this is a core of the present invention, the mist of feeding is through the separation of gas split cell, purify, with the hydrogen in the industrial waste gas and other waste gas separately, then hydrogen is passed in the hydrogen-storage jar in order to give fuel cell power generation, other waste gas is then discharged.
Described industrial waste gas (hydrogen-containing gas) hydrogen content wherein is greater than 20%, and carbon monoxide content is less than 30ppm, and sulfide content greater than this value, need be removed as impurity content (carbon monoxide and sulfide) in advance less than 2ppm.
Described PEM (PEM) is commercial perfluoro sulfonic acid membrane, and as the Nafion film of du pont company, thickness is generally 25 μ m-170 μ m.
Described gas split cell adopts the method preparation identical with common Proton Exchange Membrane Fuel Cells (PEMFC), and anode catalyst is platinum or its alloy, carrying capacity 0.2mg/cm
2-1.0mg/cm
2, cathode catalyst is platinum or its alloy, carrying capacity 0.2mg/cm
2-0.8mg/cm
2
The operating condition of described gas split cell is: be added to the direct current of each battery, voltage is 0.1V-0.5V, current density 100mA/cm
2-1000mA/cm
2, 15 ℃-90 ℃ of the running temperatures of battery, gas flow rate 1-10m/s.
Hydrogen recovery rate in the described industrial waste gas (hydrogen-containing gas) is greater than more than 60%, and single battery can improve Hydrogen Vapor Pressure 0.02-0.08MPa.
The hydrogen purity that the present invention produces is 99.5-99.99%, and every degree electricity can be produced high-purity hydrogen 1m
3-5m
3
Described fuel cell generation is meant; Fuel cell is to utilize hydrogen, and perhaps fuel such as methyl alcohol as electrolyte, under the eelctro-catalyst effect, by the electrochemical reaction of hydrogen and oxygen, produces a kind of device of electric current with PEM (PEM).As long as the external world is fuel supplying and oxygen or air continuously, just can provide lasting electric energy.Factory's excess of oxygen can be collected storage, is used for the generating of this system, so more can reach energy saving purposes.
Core work principle of the present invention is: after being provided electric energy with PEM as electrolytical battery, hydrogen is pressed the negative electrode (negative pole) that is pressurized to high pressure from the anode (positive pole) of low pressure, to finish the purpose of supercharging purifying.Key is to have utilized the hydrogen ion (H of PEM
+) selectivity and electrochemical pump principle, make the hydrogen that is recovered to have the characteristics of high-purity high pressure.It is to be noted that the electrochemistry hydrogen pump battery of structure is the same with fuel cell substantially in this invention in view of structure, mist preferably want vertical from the battery overhead stream to the bottom, can not accumulate and influence the reaction and the mobile performance of gas with the convenient water that produces.To carry out sealing around the gas diffusion layers, preventing hydrogen gas leakage, and will keep battery operated temperature as much as possible between 25-80 ℃.
The electrochemical reaction and the principle of gas split cell institute foundation are as follows among the present invention:
Anode: H
2(P
1) → 2H
++ 2e-(1)
Negative electrode: 2H
++ 2e-→ H
2(P
2) (2)
Overall reaction: H
2(P
1) → H
2(P
2) (3)
According to the Farady law, every mol electronics can produce 96484 coulomb electric charges, so the electric current of 1A can produce the hydrogen of 5.1822e-6mol/s, this is equivalent to the hydrogen of 3.1093e-4mol/min, perhaps the hydrogen of 0.006965L/min.If the voltage that each battery applies is 0.1V, the electrical power of 1W (10A) can produce the hydrogen that amounts of hydrogen is 0.06965L/min so, and every degree electricity can be produced high-purity hydrogen 4178.93L ≈ 4.2m
3
For the hydrogen purification process,
Can utilize " electrochemical pump " that hydrogen is extracted, reach the purification purpose, according to the Nernst equation:
Because p
2＞p
1So, E＜0.If battery is applied certain voltage, make hydrogen selective ground see through PEM, reach isolation of purified and hydrogen supercharging purpose.The electric energy (electrical power) that consumes depends on voltage and current, voltage and p
2/ p
1Ratio, and the overpotential size is relevant, and electric current is relevant with the amounts of hydrogen of " seeing through ".So the present invention is specially adapted to contain the waste gas recycling situation of more hydrogen.
The invention has the beneficial effects as follows: 1 uses electrochemical principle, and the hydrogen that reclaims by the gas split cell is high-purity high pressure; The course of work of 2 gas split cells and fuel cell can not produce new dusty gas, is the apparatus system of clean environment firendly; Characteristics such as 3 with respect to conventional method, has flow process short, takes up an area of and lacks, and energy consumption is low, and is simple to operate; 4 can be connected with the generating equipment of factory, directly utilize the hydrogen that reclaims to give Factory Electricity Supply, and development potentiality is very big.
Description of drawings
Fig. 1 is a hydrogen pump fundamental diagram of the present invention
Fig. 2 is hydrogen-containing gas isolation of purified of the present invention and supercharging principle schematic
Fig. 3 is a hydrogen-containing gas isolation of purified process chart of the present invention
Fig. 4 is the bipolar plate flow field figure of anode of the present invention
Figure is moved towards in gas feed of Fig. 5 battery pack and outlet
The specific embodiment
Below in conjunction with accompanying drawing embodiments of the invention are elaborated: present embodiment is being to implement under the prerequisite with the technical solution of the present invention, provided detailed embodiment and concrete operating process, but protection scope of the present invention is not limited to following embodiment.
As shown in Figure 1, the present invention has utilized the hydrogen ion (H of PEM
+) selectivity and electrochemical pump principle, the energy that provides by additional power source is extracted into or separates negative electrode to high pressure with the hydrogen in the mist from the anode of low pressure, makes the hydrogen that is recovered to have the characteristics of high-purity high pressure.It is to be noted that the electrochemistry hydrogen pump battery of structure is the same with fuel cell substantially in this invention in view of structure, mist preferably want vertical from the battery overhead stream to the bottom, can not accumulate and influence the reaction and the mobile performance of gas with the convenient water that produces.
As shown in Figure 2, hydrogen in the mist is extracted into or separates negative electrode to high pressure from the anode of low pressure, according to proton membrane technology principle, by the plural serial stage structure, progressive mode, improve Hydrogen Vapor Pressure and purity, thereby the gas outlet of a final GND in the end obtains high-purity, high pressure hydrogen.
As shown in Figure 3, industrial waste gas (mist) is earlier by the gas moistener humidification, then it directly is passed into electrochemistry hydrogen pump battery, gas split cell just. the hydrogen that is recovered to can directly feed in the hydrogen gas tank they is stored, offer fuel cell generation as high-purity hydrogen, to give Factory Electricity Supply, perhaps use as industrial chemicals.By the gas behind the gas split cell, mainly be that those non-hydrogen pneumatolytics divide and battery operated needed steam.At this moment, they are passed into the aqueous vapor knockout drum, remove moisture after, remainder of exhaust gas is discharged. the moisture of recovery enters into water storage tank, does not simultaneously have the salt solution moisturizing in water storage tank, utilizes water-circulating pump that it is passed into gas moistener, has formed a water circulation.
As shown in Figure 4, the anodal flow field of the bipolar plates in the gas split cell, the negative pole flow field becomes the mirror image symmetric relation with anodal flow field.
As shown in Figure 5, the air inlet of gas split cell moves towards figure with the gas outlet. and structure is similar with the fuel cell group, because mist want vertical from the battery overhead stream to the bottom, can not influence electrochemical reaction rates and mobile performance with the convenient water that produces because of accumulation.
Embodiment 1
Composition is H
270%, N
223%, (Ar+CH
4) 7% mist is earlier by gas moistener humidification in 85 ℃ of hot water, then it directly is passed into electrochemistry hydrogen pump battery, gas split cell just, the cell bipolar plate flow field that is used in this battery is (anodal flow field, the negative pole flow field becomes the mirror image symmetry with anodal flow field) as shown in Figure 4; Used PEM is a perfluoro sulfonic acid membrane in this battery, and thickness is 50 μ m; Used anode catalyst is a platinum in this battery, carrying capacity 0.35mg/cm
2, cathode catalyst is a platinum, carrying capacity 0.3mg/cm
2Be added to the voltage 0.3V of battery, current density 300mA/cm
2The temperature of battery remains on 80 ± 2.5 ℃, and the anode air chamber pressure is respectively 0.20MPa, negative pole air chamber pressure 0.25MPa, and hydrogen purity is greater than more than 99.99%.
Embodiment 2
Composition is with the mist (pressure is 0.20MPa) of embodiment 1, earlier by gas moistener humidification in 85 ℃ of hot water, then it directly is passed into first battery in the series connected battery group that constitutes by 3 electrochemistry hydrogen pump batteries, waste gas comes out from the positive pole of first battery, remove moisture through separation, discharging.The purified hydrogen that comes out from first GND enters the positive pole of second battery, and externally under the effect of electric field, hydrogen " infiltration " is to the negative pole of second battery, and gas pressure is increased to 0.30MPa.Hydrogen from the negative pole of second battery comes out continues supercharging at the 3rd battery, reaches 0.35MPa.The cell bipolar plate flow field that battery used of this gas split cell group is (anodal flow field, the negative pole flow field becomes the mirror image symmetry with anodal flow field) as shown in Figure 4; Used PEM is a perfluoro sulfonic acid membrane in this battery, and thickness is 50 μ m; Used anode catalyst is a platinum in this battery, carrying capacity 0.35mg/cm
2, cathode catalyst is a platinum, carrying capacity 0.3mg/cm
2Be added to the voltage 1V of battery pack, current density 300mA/cm
2The temperature of battery remains on 80 ± 2.5 ℃.The gas purity that obtains is greater than more than 99.99%, and pressure is brought up to 0.35MPa from 0.2MPa (mist).
Water under separating is recovered to water storage tank, does not have the salt solution moisturizing simultaneously in water storage tank, utilizes water-circulating pump again that it is logical as to gas moistener, has formed the circulation of a gas aqueous vapor.The high-purity high pressure hydrogen that produces in the process can directly feed in the hydrogen gas tank they are stored, and uses as high-purity hydrogen, also can be passed into it in the fuel cell pack, according to the work of fuel cell pattern, gives Factory Electricity Supply.
Embodiment 3
Composition is H
250%, CO
215%, CH
46%, (Ar+N
2) 29%, the about 5ppm of CO content, H
2The mist of the about 1.4ppm of S content (pressure is 0.25MPa) directly is passed into first battery in the series connected battery group that is made of 3 electrochemistry hydrogen pump batteries with it, and waste gas comes out from the positive pole of first battery, removes moisture through separation, discharging.The purified hydrogen that comes out from first GND enters the positive pole of second battery, and externally under the effect of electric field, hydrogen " infiltration " is to the negative pole of second battery, and gas pressure is increased to 0.35MPa.Hydrogen from the negative pole of second battery comes out continues supercharging at the 3rd battery, reaches 0.40MPa.The cell bipolar plate flow field that battery used of this gas split cell group is (anodal flow field, the negative pole flow field becomes the mirror image symmetry with anodal flow field) as shown in Figure 4; Used PEM is a perfluoro sulfonic acid membrane in this battery, and thickness is 50 μ m; Used anode catalyst is a platinum in this battery, carrying capacity 0.35mg/cm
2, cathode catalyst is a platinum, carrying capacity 0.3mg/cm
2Be added to the voltage 1.5V of battery pack, current density 320mA/cm
2The temperature of battery remains on 80 ± 2.5 ℃.The gas purity that obtains is greater than more than 99.99%, and pressure is brought up to 0.40MPa from 0.25MPa (mist).
Water under separating is recovered to water storage tank, does not have the salt solution moisturizing simultaneously in water storage tank, utilizes water-circulating pump again that it is logical as to gas moistener, has formed the circulation of a gas aqueous vapor.The high-purity high pressure hydrogen that produces in the process can directly feed in the hydrogen gas tank they are stored, and uses as high-purity hydrogen, also can be passed into them in another group fuel cell pack, according to the work of fuel cell pattern, gives Factory Electricity Supply.
Claims (7)
1. one kind is separated and purification hydrogen containing industrial waste gas method, it is characterized in that, may further comprise the steps:
The first step earlier by the gas moistener humidification, directly is passed into the gas split cell with industrial waste gas then, and the gas split cell is the plural serial stage structure that a plurality of fuel cells form, and provides electric energy to the PEM in the fuel cell pack with outer dc source;
Second step was extracted into or separated negative electrode to high pressure with the hydrogen in the industrial waste gas from the anode of low pressure, and by the plural serial stage structure, in the end the gas outlet of a GND obtains the hydrogen that pressure and purity improve;
The 3rd the step, by the gas behind the gas split cell, mainly be non-hydrogen composition and battery operated needed steam, they are passed into the aqueous vapor knockout drum, remove moisture after, remainder of exhaust gas is discharged;
In the 4th step, the moisture of recovery enters into water storage tank, does not have the salt solution moisturizing simultaneously in water storage tank, utilizes water-circulating pump that it is passed into gas moistener, has formed a water circulation.
2. separation according to claim 1 and purify the hydrogen containing industrial waste gas method is characterized in that, the hydrogen that produces in the process in second step directly feeds in the hydrogen gas tank they is stored.
3. separation according to claim 1 and purification hydrogen containing industrial waste gas method is characterized in that described industrial waste gas, hydrogen content wherein is greater than 20%, carbon monoxide content is less than 30ppm, and sulfide content is less than 2ppm, and carbon monoxide and sulfide content need be removed in advance greater than this value.
4. separation according to claim 1 and purification hydrogen containing industrial waste gas method is characterized in that described PEM is a perfluoro sulfonic acid membrane, and thickness is 25 μ m-170 μ m.
5. separation according to claim 1 and purification hydrogen containing industrial waste gas method is characterized in that described gas split cell, its anode catalyst are platinum, carrying capacity 0.2mg/cm
2-1.0mg/cm
2, cathode catalyst is a platinum, carrying capacity 0.2mg/cm
2-0.8mg/cm
2
6. separation according to claim 1 and purification hydrogen containing industrial waste gas method is characterized in that, described gas split cell, and its operating condition is: be added to the direct current of each battery, voltage is 0.1V-0.5V, current density 100mA/cm
2-1000mA/cm
2, 15 ℃-90 ℃ of the temperature of battery, gas flow rate 1m/s-10m/s.
7. separation according to claim 1 and purify the hydrogen containing industrial waste gas method is characterized in that, described industrial waste gas vertical from gas split cell overhead stream to the bottom.
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| CN114684788B (en) * | 2020-12-29 | 2023-07-07 | 中石化石油工程技术服务有限公司 | Hydrogen separation and purification device and method for hydrogen-containing mixed gas |
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