CN104030245A - Hydrogen purifying method and device for refinery dry gas after recovery of light olefins with high yield and high purity - Google Patents
Hydrogen purifying method and device for refinery dry gas after recovery of light olefins with high yield and high purity Download PDFInfo
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- CN104030245A CN104030245A CN201410220909.8A CN201410220909A CN104030245A CN 104030245 A CN104030245 A CN 104030245A CN 201410220909 A CN201410220909 A CN 201410220909A CN 104030245 A CN104030245 A CN 104030245A
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Abstract
The invention relates to a hydrogen purifying method for refinery dry gas after recovery of light olefins with high yield and high purity. The method comprises the following steps: S1, first section membrane separation; S2, primary pressure swing adsorption; S3, second pressure swing adsorption; S4, second section membrane separation. The invention further relates to a hydrogen purifying device for refinery dry gas after recovery of light olefins with high yield and high purity. The device comprises a first membrane separating device, a second membrane separating device, a first pressure swing adsorption tower, a second pressure swing adsorption tower and first and second pressurizing devices. According to the hydrogen purifying method and device for refinery dry gas after recovery of light olefins with high yield and high purity provided by the invention, by adopting a technology combining pressure swing adsorption and membrane separation, the deficiencies on purity and low recovery rate of the two processes are remedied, so that hydrogen in the refinery dry gas after recovery of light olefins is recovered with high yield and purity, and the residual gas after hydrogen recovery can directly enter a burning gas pipe network to combust.
Description
Technical field
The invention belongs to chemical separating and chemical machinery field, relate to and a kind of reclaim after light olefin high yield high purity in oil refinery dry gas and carry hydrogen methods and device.
Background technology
Useful component in oil refinery dry gas is mainly hydrogen, light olefin and light alkane etc.These components are all of great value in refinery, but they still do not realize optimum use very in a large number at present, but have directly been used as fuel, the even direct ignition torch emptying having.For the catalytic cracked dry gas of the amount of accounting for maximum in oil refinery dry gas, both contained hydrogen, also contain a large amount of light olefins and light alkane.These components can be separated respectively and utilize, higher than the raw material benefit that it is directly used as to fuel or reformation hydrogen production, synthesizing methanol.
Oil refinery dry gas reclaims light olefin several different methods at present, such as low temperature separation process etc., belong to the prior art of finding broad application, in oil refinery dry gas, light olefin content is conventionally in 10-40% volume percent, residual gas is hydrogen, nitrogen and methane, although can obtain heat by burning residual gas, hydrogen can use as hydrogenation in refinery, price is higher, also uneconomical as the mode of fuel gas burning.The hydrogen that also contains about 40-80% in the oil refinery dry gas reclaiming after light olefin, economic worth be can not ignore.
At present to wherein a large amount of hydrogen of dry-gas recovery after recovery light olefin, can adopt the methods such as membrane separation process, pressure-variable adsorption, low temperature separation process, but, the hydrogen purity reclaiming by membrane separation process is not high, be generally below 95%, because purity directly has influence on the price of hydrogen, therefore membrane separation process economic worth is little.And the hydrogen psa rate of recovery is on the low side, conventionally only have 85%, low temperature separation process, due to a large amount of colds of needs, adopt low temperature separation process cost too expensive, and the hydrogen purity that low temperature separation process obtains is not high to hydrogen.
Summary of the invention
For overcome prior art exist the rate of recovery low or reclaim purity low, the technological deficiency of deficiency in economic performance, after the open a kind of recovery light olefin of the present invention, in oil refinery dry gas, high yield high purity is carried hydrogen methods and device, and the oil refinery dry gas reclaiming after light olefin is carried out to hydrogen recovery.
After recovery light olefin of the present invention, in oil refinery dry gas, high yield high purity is carried hydrogen methods, comprises the steps:
One section of membrane sepn of step 1.: unstripped gas enters the first membrane separation unit, infiltration gas enter step 2, impermeable gas with
After mixing, the stripping gas pressurization of subsequent step 2 to 3 enters step 4;
Step 2. one-level pressure-variable adsorption: in step 1, the infiltration gas of the first membrane separation unit enters the first pressure-swing absorber, the
The non-stripping gas of one pressure-swing absorber enters step 3, and stripping gas enters step 4 after mixing with the stripping gas pressurization of step 1 impermeable gas, subsequent step 3;
Step 3. secondary pressure-variable adsorption: the non-stripping gas in step 2 enters the second pressure-swing absorber, the second pressure-swing absorber
Non-stripping gas export as product hydrogen, stripping gas mix with step 1 impermeable gas, step 2 stripping gas pressurization after enter step 4;
Step 4. two-segment film separates: the solution of first, second pressure-swing absorber output in step 1 impermeable gas, step 2,3
Air-breathingly after mixing pressurization, enter the second membrane separation unit, enter the first membrane separation unit together with after the infiltration gas of the second membrane separation unit turns back in step 1 and to mix with unstripped gas pressurization.
Preferably, the impermeable gas that the membrane separation unit in described step 4 obtains directly enters refinery's burning gas pipe network.
Preferably, before described step 1 Raw gas enters the first membrane separation unit, also comprise pressurization steps.
Further, in described step 1, unstripped gas is forced into 1.5-3 MPa, unstripped gas is forced into 1.5-3 MPa, in described step 4, be forced into 1-2 MPa.
Preferably, described step 1 is normal temperature to service temperature in 4, and described normal temperature is 0-40 degree Celsius of scope.
After recovery lighter hydrocarbons of the present invention, in oil refinery dry gas, high yield high purity is carried hydrogen production device, comprises the first membrane separation unit, the second membrane separation unit, the first pressure-swing absorber, the second pressure-swing absorber and the first pressurizing device and the second pressurizing device;
The per-meate side of described the first membrane separation unit is connected with the import of the first pressure-swing absorber, its non-per-meate side is connected with the import of the second membrane separation unit through the second pressurizing device, the per-meate side of described the second membrane separation unit is mixed and is connected with the import of the first membrane separation unit by the first pressurizing device with unstripped gas, the non-stripping gas outlet of tower top of described the first pressure-swing absorber is connected with the import of the second pressure-swing absorber, at the bottom of its tower, stripping gas is connected with the import of the second membrane separation unit through the second pressurizing device, the overhead streams of described the second pressure-swing absorber goes out product hydrogen, at the bottom of its tower, stripping gas outlet is connected with the import of the second membrane separation unit by the second pressurizing device.
Preferably, the non-per-meate side outlet of described the second membrane separation unit is connected with refinery's burning gas pipe network.
Adopt after recovery light olefin of the present invention high yield high purity in oil refinery dry gas to carry hydrogen methods and device, adopt two sections
Pressure-variable adsorption, two-segment film separate the technology of the two combination, two kinds of purity and low defects of the rate of recovery that technique exists are separately made up, realize the high yield to reclaiming hydrogen in the oil refinery dry gas after light olefin, highly purified recovery, the residual gas after recover hydrogen can directly enter refinery's burning gas pipe network burning.
Brief description of the drawings
Fig. 1 illustrates after recovery light olefin of the present invention that high yield high purity in oil refinery dry gas carries a kind of embodiment schematic diagram of hydrogen methods;
Fig. 2 illustrates after recovery light olefin of the present invention that high yield high purity in oil refinery dry gas carries a kind of embodiment schematic diagram of hydrogen production device;
In each figure, Reference numeral name is called: 1-first pressurizing device 2-second pressurizing device 3-first pressure-swing absorber 4-second pressure-swing absorber 5-first membrane separation unit 6-the second membrane separation unit 7-refinery burning gas pipe network.
Embodiment
Below in conjunction with accompanying drawing, the specific embodiment of the present invention is described in further detail.
In prior art, after the light olefins such as the methane in oil refinery dry gas, ethene, ethane are reclaimed, the main component of remaining gas is that about 30-60%H2,5-15%N2,5-24% methane, all the other components add up to and are no more than 1%, and the percentage composition in this specification sheets is volume percent.
Reclaim hydrogen component maximum in the oil refinery dry gas after light olefin, next is methane, hydrogen is as conventional oil refining hydrogenation, and directly burn very unfortunate as burning gas, the present invention provides a kind of for this reason and reclaims after light olefin high yield high purity in oil refinery dry gas and carry hydrogen methods, comprises the steps: one section of membrane sepn of step 1.: unstripped gas enters the first membrane sepn
Device, infiltration gas enters step 2, and impermeable gas enters step 4 after mixing with the stripping gas pressurization of follow-up two steps; Step 2. one-level pressure-variable adsorption: in step 1, the infiltration gas of the first membrane separation unit enters the first pressure-swing absorber, the non-stripping gas of the first pressure-swing absorber enters step 3, and stripping gas enters step 4 after mixing with the stripping gas pressurization of step 1 impermeable gas, a follow-up step; Step 3. secondary pressure-variable adsorption: the non-stripping gas in step 2 enters the second pressure-swing absorber, the non-stripping gas of the second pressure-swing absorber is exported as product hydrogen, and stripping gas enters step 4 mix pressurization with step 1 impermeable gas, step 2 stripping gas after; Step 4. two-segment film separation: in step 1 impermeable gas, step 2,3, the stripping gas of first, second pressure-swing absorber output enters the second membrane separation unit after mixing pressurization, the infiltration gas of the second membrane separation unit turns back in step 1 and enter the first membrane separation unit together with after unstripped gas pressurization mixing.
Oil refinery dry gas after recovery light olefin enters the first membrane separation unit as unstripped gas hydrogen is carried out to membrane sepn for the first time, and the first membrane separation unit is preferably pi film, and in the infiltration gas after separation, hydrogen purity is promoted to 60%-80%
Still contain a small amount of methane and nitrogen, the infiltration gas of the first membrane separation unit enters the first pressure-swing absorber hydrogen is further purified, its impermeable gas still contains more hydrogen, enters the second membrane separation unit and continue concentrated hydrogen through mix pressurization with first, second pressure-swing absorber stripping gas after; The non-stripping gas that the first pressure-swing absorber obtains enters the second pressure-swing absorber, stripping gas enters the concentrated hydrogen of the second membrane separation unit continuation mix pressurization with impermeable gas, the second pressure-swing absorber stripping gas of the first membrane separation unit after, to improve the rate of recovery of hydrogen.The second pressure-swing absorber absorbs after the non-stripping gas of the first pressure-swing absorber, directly export highly purified hydrogen as product hydrogen from the non-stripping gas exit of the second pressure-swing absorber, the stripping gas warp of the second pressure-swing absorber output and the impermeable gas of the first film device, the first pressure-swing absorber stripping gas enters the second membrane separation unit after mixing pressurization, now in the stripping gas of the second pressure-swing absorber output, still contain the hydrogen component of about 6-15%, for further improving hydrogen yield, these gases are entered to the second membrane separation unit after pressurization to be separated, preferably polyester film of the second membrane separation unit, together with after mixing pressurization with unstripped gas after hydrogen component purity is wherein improved, enter the first membrane separation unit and repeat the recovery to hydrogen component.
The present invention adopts the array mode of membrane sepn+bis-section pressure-variable adsorption+membrane sepn, the hydrogen component reclaiming in the oil refinery dry gas after light olefin is reclaimed, utilize the array mode of membrane sepn and pressure-variable adsorption, the stripping gas of one-level membrane sepn impermeable gas, two-stage pressure-swing absorber all comes back to participation circulation in system and absorbs, hydrogen is repeatedly purified and juice circulation hydrogen mode, improved yield and the purity of hydrogen.
Preferably, the impermeable gas that the membrane separation unit in described step 4 obtains is because hydrogen is absorbed by major part, and residual gas is that methane is main, also contain the gas of part nitrogen and lighter hydrocarbons, calorific value is higher, can directly enter refinery's burning gas pipe network, uses as refinery's fuel gas.
The dry gas reclaiming after light olefin generally all carries larger pressure, can be without pressurization, if but dry gas due to the system of expanding
The words that the mode such as cold has been depressurized, can before entering the first membrane separation unit, unstripped gas pressurize, pressurization scope can be chosen in 1.5 to 3 MPas, the first membrane separation unit is exported impermeable gas with pressure, pressurization scope while entering the second membrane separation unit after mixing pressurization with the stripping gas of first, second pressure-swing absorber output can be chosen in 1-2 MPa, subsequent film is separated to osmotic effect better.In whole sepn process, membrane sepn or pressure-variable adsorption, can carry out all without harsh requirement at normal temperatures to temperature, need not heat or freeze, and have saved the energy and equipment.A kind of embodiment of the present invention shown in Fig. 1, has comprised that above-mentioned pressurization steps and the impermeable gas by the second membrane separation unit send into the step of refinery's gas ductwork.
For realizing aforesaid method, the invention provides and a kind of reclaim after light olefin high yield high purity in oil refinery dry gas and carry hydrogen production device, as shown in Figure 2, comprise the first membrane separation unit 5, the second membrane separation unit 6, the first pressure-swing absorber 3, the second pressure-swing absorber 4 and the first pressurizing device 2; The per-meate side of described the first membrane separation unit 5, the second membrane separation unit 6 is all connected with the import of the first pressure-swing absorber 3, at the bottom of the non-stripping gas outlet of the tower top of described the first pressure-swing absorber 3 and tower, stripping gas outlet is connected with the import of the second pressure-swing absorber 4 and the first membrane separation unit 5 respectively, and at the bottom of the tower of described the second pressure-swing absorber 4, stripping gas exports and passes through the first pressurizing device 2 and be connected with the import of the second membrane separation unit 6.The first membrane separation unit is the film of the saturating hydrogen of high pressure, for example polymeric amide hydrogen film, and the second membrane separation unit is low pressure permeable hydrogen membrane, for example polycarbonate hydrogen film.
After recovery light olefin, in oil refinery dry gas, high yield high purity is carried hydrogen production device, preferred, and the non-per-meate side outlet of described the first membrane separation unit and the second membrane separation unit is all connected with refinery's burning gas pipe network 7.
For realizing aforesaid preferred pressurization steps, the import of described the first membrane separation unit is also connected with the second pressurizing device 1.
Below provide some specific embodiments of the present invention:
Embodiment 1. unstripped gas hydrogen 40%, methane 50%, nitrogen and remaining gas 10%, pressure 1.5 MPas, 30 degrees Celsius of temperature, with 10,000Nm
3/ h flow is sent in device as shown in Figure 2, unstripped gas is forced into 3 MPas through the first pressurizing device, enter the first membrane separation unit, wherein the first membrane separation unit adopts polyamide membrane assembly, it is main that the first pressure-swing absorber is filled with the sorbent material such as gac and aluminum oxide, the second pressure-swing absorber is filled with essence, and to carry the adsorbent of molecular sieve of hydrogen be main, and the second membrane separation unit adopts polycarbonate membrane module, and the second pressurizing device is forced into 2 MPas to the stripping gas of the second pressure-swing absorber;
Measuring the rate of recovery of hydrogen is 99%, and recover hydrogen purity is more than 99.99%.
Embodiment 2. unstripped gas hydrogen 60%, methane 25%, nitrogen and remaining gas 15%, pressure 2.5 MPas, 30 degrees Celsius of temperature, with 10,000Nm
3/ h flow is sent in device as shown in Figure 2, unstripped gas directly enters the first membrane separation unit, wherein the first membrane separation unit adopts polyamide membrane assembly, it is main that the first pressure-swing absorber is filled with the sorbent material such as gac and aluminum oxide, the second pressure-swing absorber is filled with essence, and to carry the adsorbent of molecular sieve of hydrogen be main, the second membrane separation unit adopts polycarbonate membrane module, and the second pressurizing device is forced into 1.2 MPas to the stripping gas of the second pressure-swing absorber;
Measuring the rate of recovery of hydrogen is 99%, and recover hydrogen purity is more than 99.99%.
Embodiment 3. unstripped gas hydrogen 75%, methane 20%, nitrogen and remaining gas 5%, pressure 1 MPa, 25 degrees Celsius of temperature, with 10,000Nm
3/ h flow is sent in device as shown in Figure 2, unstripped gas is forced into 3 MPas through the first pressurizing device, enter the first membrane separation unit, wherein the first membrane separation unit adopts polyamide membrane assembly, it is main that the first pressure-swing absorber is filled with the sorbent material such as gac and aluminum oxide, the second pressure-swing absorber is filled with essence, and to carry the adsorbent of molecular sieve of hydrogen be main, and the second membrane separation unit adopts polycarbonate membrane module, and the second pressurizing device is forced into 1 MPa to the stripping gas of the second pressure-swing absorber;
Measuring the rate of recovery of hydrogen is 99%, and recover hydrogen purity is more than 99.99%.
Embodiment 4. unstripped gas hydrogen 80%, methane 10%, nitrogen and remaining gas 10%, pressure 2 MPas, 25 degrees Celsius of temperature, with 10,000Nm
3/ h flow is sent in device as shown in Figure 2, unstripped gas directly enters the first membrane separation unit, wherein the first membrane separation unit adopts polyamide membrane assembly, it is main that the first pressure-swing absorber is filled with the sorbent material such as gac and aluminum oxide, the second pressure-swing absorber is filled with essence, and to carry the adsorbent of molecular sieve of hydrogen be main, the second membrane separation unit adopts polycarbonate membrane module, and the second pressurizing device is forced into 1.5 MPas to the stripping gas of the second pressure-swing absorber;
Measuring the rate of recovery of hydrogen is 99%, and recover hydrogen purity is more than 99.99%.
Previously described is each preferred embodiment of the present invention, preferred implementation in each preferred embodiment is if not obviously contradictory or taking a certain preferred implementation as prerequisite, each preferred implementation arbitrarily stack combinations is used, design parameter in described embodiment and embodiment is only the invention proof procedure for clear statement contriver, not in order to limit scope of patent protection of the present invention, scope of patent protection of the present invention is still as the criterion with its claims, the equivalent structure that every utilization specification sheets of the present invention and accompanying drawing content are done changes, in like manner all should be included in protection scope of the present invention.
Claims (6)
1. after recovery light olefin, in oil refinery dry gas, high yield high purity is carried hydrogen methods, comprises the steps:
One section of membrane sepn of step 1.: unstripped gas enters the first membrane separation unit, infiltration gas enter step 2, impermeable gas with
After mixing, the stripping gas pressurization of subsequent step 2 to 3 enters step 4;
Step 2. one-level pressure-variable adsorption: in step 1, the infiltration gas of the first membrane separation unit enters the first pressure-swing absorber, the
The non-stripping gas of one pressure-swing absorber enters step 3, and stripping gas enters step 4 after mixing with the stripping gas pressurization of step 1 impermeable gas, subsequent step 3;
Step 3. secondary pressure-variable adsorption: the non-stripping gas in step 2 enters the second pressure-swing absorber, the second pressure-swing absorber
Non-stripping gas export as product hydrogen, stripping gas mix with step 1 impermeable gas, step 2 stripping gas pressurization after enter step 4;
Step 4. two-segment film separates: the solution of first, second pressure-swing absorber output in step 1 impermeable gas, step 2,3
Air-breathingly after mixing pressurization, enter the second membrane separation unit, enter the first membrane separation unit together with after the infiltration gas of the second membrane separation unit turns back in step 1 and to mix with unstripped gas pressurization.
2. reclaim as claimed in claim 1 after light olefin high yield high purity in oil refinery dry gas and carry hydrogen methods, it is characterized in that, the impermeable gas that the membrane separation unit in described step 4 obtains directly enters refinery's burning gas pipe network.
3. reclaim as claimed in claim 1 after light olefin high yield high purity in oil refinery dry gas and carry hydrogen methods, it is characterized in that, before described step 1 Raw gas enters the first membrane separation unit, also comprise pressurization steps, unstripped gas is forced into 1.5-3 MPa, in described step 4, be forced into 1-2 MPa.
4. reclaim as claimed in claim 1 after light olefin high yield high purity in oil refinery dry gas and carry hydrogen methods, it is characterized in that, described step 1 is normal temperature to service temperature in 4, and described normal temperature is 0-40 degree Celsius of scope.
5. after recovery light olefin, in oil refinery dry gas, high yield high purity is carried hydrogen production device, it is characterized in that, comprise the first membrane separation unit (5), the second membrane separation unit (6), the first pressure-swing absorber (3), the second pressure-swing absorber (4) and the first pressurizing device (1) and the second pressurizing device (2);
The per-meate side of described the first membrane separation unit (5) is connected with the import of the first pressure-swing absorber (3), its non-per-meate side is connected with the import of the second membrane separation unit through the second pressurizing device (2), the per-meate side of described the second membrane separation unit (6) is mixed and is connected with the import of the first membrane separation unit (5) by the first pressurizing device (1) with unstripped gas, the non-stripping gas outlet of tower top of described the first pressure-swing absorber (3) is connected with the import of the second pressure-swing absorber (4), at the bottom of its tower, stripping gas is connected with the import of the second membrane separation unit (6) through the second pressurizing device (2), the overhead streams of described the second pressure-swing absorber (4) goes out product hydrogen, at the bottom of its tower, stripping gas outlet is connected with the import of the second membrane separation unit (6) by the second pressurizing device (2).
6. after recovery light olefin, in oil refinery dry gas, high yield high purity is carried hydrogen production device, it is characterized in that, the non-per-meate side outlet of described the second membrane separation unit is connected with refinery's burning gas pipe network (7).
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CN104495752A (en) * | 2014-12-31 | 2015-04-08 | 中国石油天然气股份有限公司 | Method and system for jointly treating refinery gas by adopting membrane separation and pressure swing adsorption |
CN104986735A (en) * | 2015-07-17 | 2015-10-21 | 四川天一科技股份有限公司 | Method for improving hydrogen recovery rate |
CN113731127A (en) * | 2020-05-29 | 2021-12-03 | 中国石油化工股份有限公司 | Process for recovering light hydrocarbon from hydrogen-containing gas in refinery |
CN114751376A (en) * | 2022-03-31 | 2022-07-15 | 国家能源集团宁夏煤业有限责任公司 | Separation method of synthesis tail gas |
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CN203513271U (en) * | 2013-10-30 | 2014-04-02 | 四川天采科技有限责任公司 | High-yield and high-purity device for producing hydrogen through reforming and converting refinery dry gas |
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Publication number | Priority date | Publication date | Assignee | Title |
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CN104495752A (en) * | 2014-12-31 | 2015-04-08 | 中国石油天然气股份有限公司 | Method and system for jointly treating refinery gas by adopting membrane separation and pressure swing adsorption |
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CN113731127A (en) * | 2020-05-29 | 2021-12-03 | 中国石油化工股份有限公司 | Process for recovering light hydrocarbon from hydrogen-containing gas in refinery |
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CN114751376B (en) * | 2022-03-31 | 2024-01-12 | 国家能源集团宁夏煤业有限责任公司 | Separation method of synthetic tail gas |
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