CN101773765B - Method for reclaiming hydrogen in refinery dry gas - Google Patents
Method for reclaiming hydrogen in refinery dry gas Download PDFInfo
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- CN101773765B CN101773765B CN2010100005914A CN201010000591A CN101773765B CN 101773765 B CN101773765 B CN 101773765B CN 2010100005914 A CN2010100005914 A CN 2010100005914A CN 201010000591 A CN201010000591 A CN 201010000591A CN 101773765 B CN101773765 B CN 101773765B
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Abstract
The invention discloses a method for reclaiming hydrogen in refinery dry gas, which comprises the following steps: (1) firstly, pre-separating the refinery dry gas in which the molar content of the hydrogen is 20 to 35 percent and the pressure is not lower than 0.8MPa by using a membrane separation unit so as to enrich H2 in the refinery dry gas on the permeation side of a membrane; (2) secondly, pressurizing the gas rich in hydrogen after enriching on the permeation side of the membrane in the membrane separation unit to 1.0 to 1.2MPa, and feeding the gas into a pressure swing adsorption unit; and (3) finally, further adsorbing the hydrocarbons contained in the gas by using the pressure swing adsorption unit to ensure that the purity of the H2 reaches 95 to 99.5 percent based on mole percent and the pressure is kept between 0.9 and 1.1MPa, and delivering the hydrocarbons serving as hydrogen products. The method mainly comprises the membrane separation unit and the pressure swing adsorption unit. The method can purify the hydrogen in the refinery dry gas in which the molar content of the hydrogen is 20 to 35 percent to over 95 percent so as to fully reclaim the hydrogen resources.
Description
Technical field
The present invention relates to recover hydrogen (H from oil refinery dry gas
2: the method for 20mol%～35mol%) is a kind of method of adsorbing integrated technique recover hydrogen from oil refinery dry gas through film separations/transformation.
Background technology
Refinery gas is mainly derived from the crude oil secondary operations, like the gas that produces in the processes such as catalytic cracking, thermal cracking, time-delay coking, hydrocracking.5% of its output average out to crude runs mainly contains components such as hydrogen, methane, ethene, ethane, propylene, propane, is a kind of valuable source of petrochemical industry.The catalytic cracked dry gas amount is maximum in China's refinery gas, recycles because of no appropriate method in the past, can only act as a fuel and burn in vain, causes huge waste.Contain a large amount of hydrogen in China's refinery gas, as refining at gasoline and diesel hydrogenation, in the processing procedures such as lube oil hydrogenation, the hydrogen content that has in the discharge tail gas is up to 80% (mol%); Hydrogen content in the catalytic cracked dry gas is generally at 20%～50% (mol%).The recycling of hydrogen in these tail gas not only can significantly reduce the consumption of hydrogen feedstock, reduces the hydrogen manufacturing cost, and the recycling of realizing refinery gas is all had very significant meaning.
Transformation adsorbed gas isolation technics (PSA) is to rely on the variation of pressure to realize absorption and the regeneration of gas, has characteristics such as reproduction speed is fast, energy consumption is low, simple to operate, stable.China introduces external PSA since early 1980s and puies forward the hydrogen technology, like the Shanghai petrochemical industry, raise sub-petrochemical industry, Maoming petrochemical industry, Liaoyang chemical fibre etc.Since early 1990s the PSA technology developed voluntarily of China be used for the recovery of refinery gas hydrogen.At present, the PSA technology of China is ripe, and for the hydroforming gas of PETROLEUM PROCESSING enterprise of the tens of family of China and catalytic cracked dry gas etc. provide the hydrogen recovery service, production scale can substitute import fully in continuous expansion.The PSA method has two advantages: the one, and high to the removal efficiency of impurity, can satisfy the requirement of any technology, the 2nd, can produce high-purity hydrogen.This method is applicable to from hydrogen concentration greater than extracting the higher hydrogen-rich gas of concentration the unstripped gas of 40% (mol%).Can be more than the hydrogen upgrading to 99.9% (mol%); Hydrogen recovery rate is about about 85%～90%.And because hydrogen is non-stripping gas, when the content lower (being lower than 40%) of hydrogen, make that the amount of the adsorbent that PSA needs is very big, thereby investment, occupation of land, the energy consumption of device are all corresponding bigger.
Membrane separation technique has been widely used in ethene, propylene, lighter hydrocarbons, oil gas and hydrogen recovery; China reclaims nearly 30 covers of device of hydrogen in the refinery gas, adopts membrane technology at refinery's low pressure (existing application example of recover hydrogen in the dry gas of 0.8MPa～1.2MPa) especially over the past two years.Membrane separation process is applicable to from hydrogen concentration greater than extracting the higher hydrogen-rich gas of concentration the refinery gas of 35% (mol%).Can be according to the composition of unstripped gas, hydrogen upgrading to 90%～99% (mol%); Hydrogen recovery rate is about 80%～90% (mol%).The gas film separating technology have take up an area of little, energy consumption is low, simple operation and other advantages.
Adopt membrane separation technique separately; Be not suitable for and density of hydrogen in the oil refinery dry gas be lower than hydrogen reclaims in the gas of 35% (mol%); Be difficult to carry dense to more than 90% (mol%); If but utilize transformation adsorbed gas isolation technics to reclaim the hydrogen of this concentration separately, and invest hugely, lost the economic implications of recover hydrogen.Therefore the hydrogen that is lower than in the oil refinery dry gas of 35% (mol%) for hydrogen concentration does not at present also have cost-effective recovering means.
Summary of the invention
The object of the present invention is to provide the recovery technology of hydrogen in a kind of oil refinery dry gas, utilizing this technology can be more than the hydrogen upgrading to 95% (mol%) in the oil refinery dry gas of 20%～35% (mol%) with hydrogen concentration.
The technical scheme that the present invention adopts is the reclaiming hydrogen in refinery dry gas of integrated film separation and adsorption gas separating technology, and its process is:
(1) at first, utilizing film separation unit is that 20%～35% oil refinery dry gas carries out pre-separation with the hydrogen molar content, makes H2 in the oil refinery dry gas be enriched in the per-meate side (membrane permeate gas) of film;
(2) then, the gas pressurized that is rich in hydrogen after the per-meate side enrichment of film in the film separation unit behind 1.0MPa～1.2MPa, is got into psa unit;
(3) last, utilize the hydro carbons that contains in the further adsorbed gas of psa unit, make H
2Purity reach 95%～99.5% by mole percentage, pressure remains on 0.9MPa～1.1MPa, sees off as hydrogen product.
Oil refinery dry gas also carried out demist before advancing film separation unit handles to remove condensable liquid.Also need carry out filtration treatment to remove particle, avoid the film in the polluted membrane unit greater than 0.01 μ m.Oil refinery dry gas also need be preheated to earlier more than the dew-point temperature before getting into film separation unit, avoids the infringement of liquid hydrocarbon to film.
Film in film separation unit oozes stripping gas in residual air and the psa unit can be sent into the gas pipe network as tail gas and focus on.
Film separates and pressure swing adsorption all has its best applications scope, optimum technique for applying; Though it is unsatisfactory or economical inadequately no matter to be that membrane separation technique or pressure swing adsorption are lower than the refining effect of hydrogen in 35% the oil refinery dry gas for density of hydrogen; But the present invention utilizes film separation/pressure swing adsorption organic integration technology can give full play to the advantage of each monotechnics; Can the hydrogen recovery that original density of hydrogen is lower than in 35% the oil refinery dry gas be purified to 95% (mol%); Be the effective technology means that solve the oil refinery dry gas resource, can enlarge the range of application of from oil refinery dry gas, extracting hydrogen, resource is utilized effectively.
Description of drawings
Fig. 1 is certain factory's film separation/transformation adsorbing integration technology hydrogen recovery technological process and material balance sketch map.
The specific embodiment
The calculated examples of the comprehensive reutilization through certain plant catalytic dry gas describes in further detail the present invention below.
Hydrogen content is molar percentage in the following calculated examples:
At present, certain refinery's three catalysis drying gas amount is 141.4t/d (7000Nm
3/ h), all getting into the gas pipe network, four catalysis drying gas amounts are 482.4t/d (25000Nm
3/ h), wherein there is 295t/d to advance triphen, 187.4t/d gets into the gas pipe network; According to the too high problem of the present hydrogen manufacturing cost of the said firm, with the hydrogen recovery utilization in three catalysis, four catalysis drying gas, with minimizing hydrogen feedstock consumption and reduction hydrogen cost, and assurance reaches the purity (hydrogen purity>=95%) of customer requirements hydrogen.
Concrete technological process is as shown in Figure 1:
Three catalysis, four catalysis drying gas at first carry out demist and filter: promptly earlier get into demister respectively and carry out demist, remove most of condensable liquid; The gas that demister comes out gets into two-stage filter respectively, reaches the particle greater than 0.01 μ m further to remove mist of oil.Dry gas through after the demist filtration is heated to 75 ℃ through preheater with unstripped gas respectively again, makes unstripped gas away from dew point.The gas that heated gets into membrane separator through tubular filter to be separated, and at low-pressure side generation hydrogen, it is 84.5% through film separation back hydrogen content that three catalysis drying gas reach 77.2%, four catalysis drying gas through film separation back hydrogen content.The gas that is rich in hydrogen that separates the back low-pressure side through film of three catalysis and four catalysis is pressurized to 1.2MPa again through compressor and advances VPSA Vacuum Pressure Swing Adsorption recovery hydrogen production device.Tail gas after three catalysis drying gas separate through film advances the gas pipeline, and the tail gas after four catalysis drying gas separate through film advances gas pipeline and triphen respectively.
Refinery gas amounts to the about 8379.1Nm of recyclable hydrogen after film separation/transformation absorption integrated technique is handled
3/ h, recover hydrogen purity>=95%, pressure 1.15MPa.The VPSA stripping gas advances the gas pipeline.
The result of each burst parameter of materials comprises that film separates and transformation absorption two parts, lists table 1 and table 2 respectively in.
Table 1 film separating part result
Three catalysis:
Four catalysis:
Table 2 Vacuum Pressure Swing Adsorption result
Explain: 1. because hydrogen sulfide adopts dry method to deviate from, this mass balance calculates.
2. to the material in the diesel oil hydrogenation tail gas, divide carbon four and carbon five saturated and unsaturated adding together to calculate.
Can know that by last table three, four catalysis drying gas separate/transformation absorption integrated technique recyclable hydrogen 8379Nm with diesel oil hydrogenation tail gas through film
3/ h (hydrogen purity>=95%), gross investment about 2,700 ten thousand (not containing booster pump and civil engineering expense), device builds up the back operation and can recoup capital outlay less than 1 year.
Utilize film to separate to anticipate catalysis drying gas, not only raw hydrogen concentration and has guaranteed that hydro carbons tail gas does not need supercharging can directly advance the triphen device in the optimum operation scope of PSA, and integrated coupling effect is remarkable.
Technological merit
(1) be applicable to hydrogen content at 20%～35% oil refinery dry gas, hydrogen recovery rate is with to reclaim concentration all higher
Hydrogen content after reclaiming with membrane separation process separately, under the situation that guarantees certain rate of recovery, can only bring up to 60%～80% with density of hydrogen at 20%～35% oil refinery dry gas, can not directly be used as hydrogen product.And separately with the method recovery of PSA, because hydrogen is non-stripping gas, the content of hydrogen is low, make that the amount of the adsorbent that PSA needs is very big, thereby investment, occupation of land, the energy consumption of device is all corresponding bigger.And utilize film separation/transformation absorption integrated technique, and hydrogen recovery rate is reached more than 80%, recover hydrogen concentration reaches more than 95%, can meet the needs of production fully, and small investment, energy consumption is low.
(2) small investment, the total system energy consumption is lower
Integrated technique can make full use of the pressure of oil refinery dry gas self and realize membrane separating.At film separation unit, have only preprocessing part, purging and instrument partly to need power consumption seldom.Secondly, through film separation unit, the density of hydrogen of gas brings up to 70%～85% from 20%～35%, and tolerance is about 1/3rd of unstripped gas, gets into psa unit again.The raising of density of hydrogen, the minimizing of tolerance make the scale, investment, occupation of land, energy consumption etc. of consumption, psa unit of adsorbent all reduce greatly; At psa unit, because the hydrogen that reclaims is non-desorption gas, the pressure loss is very little, does not need compressor boost or increase pressure seldom just can directly get into the hydrogen pipe network; And ooze residual air (tolerance be about unstripped gas 2/3rds) through what film separation unit separated, almost not loss of pressure can directly get into the gas pipe network or as the raw material of styrene device.
(3) simple to operate, operating cost is low
Equipment is simple and safe, easy to operate, occupation of land is little, and operating cost is low, does not have new pollutant to produce.According to the purity requirement of density of hydrogen, product hydrogen in material gas quantity, unstripped gas square one not, can realize through regulating methods such as membrane operations parameter.
(4) remarkable in economical benefits
Utilize film separation/transformation absorption integrated technique that the hydrogen of hydrogen content in 20%～35% oil refinery dry gas is reclaimed; And as the hydrogen product utilization; Avoid a large amount of wastes of hydrogen, significantly reduced the consumption of hydrogen feedstock in the refinery, reduced the hydrogen cost; It was recoverable fully invested in 1 year that remarkable in economical benefits, device are built up the back operation.
Claims (4)
1. reclaiming hydrogen in refinery dry gas, its process is:
(1) at first, utilizing film separation unit is that 20%～35% oil refinery dry gas carries out pre-separation with the hydrogen molar content, makes the H in the oil refinery dry gas
2Be enriched in the per-meate side of film;
(2) then, the gas pressurized that is rich in hydrogen after the per-meate side enrichment of film in the film separation unit behind 1.0MPa～1.2MPa, is got into the Vacuum Pressure Swing Adsorption unit;
(3) last, utilize in the Vacuum Pressure Swing Adsorption unit hydro carbons that contains in the further adsorbed gas, make H
2Purity reach 95%～99.5% by mole percentage, pressure remains on 0.9MPa～1.1MPa, sees off as hydrogen product.
2. the method for claim 1 is characterized in that: said oil refinery dry gas also carried out demist before advancing film separation unit handles to remove condensable liquid.
3. method as claimed in claim 2 is characterized in that: described oil refinery dry gas also carries out filtration treatment to remove the particle greater than 0.01 μ m after handling through described demist and before advancing film separation unit.
4. method as claimed in claim 3 is characterized in that: said oil refinery dry gas also is preheated to more than the dew-point temperature earlier after the described filtration treatment of process and before getting into film separation unit.
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| CN101905112A (en) * | 2010-09-03 | 2010-12-08 | 魏伯卿 | Method and device for separating hydrogen and hydrocarbon in petroleum drying gas by using multi-stage cascade temperature-changing membrane |
| CN103552984A (en) * | 2013-10-30 | 2014-02-05 | 四川天采科技有限责任公司 | Method for producing hydrogen with high yield and high purity by reforming and transforming dry refinery gas |
| CN104030245B (en) * | 2014-05-23 | 2016-06-01 | 四川天采科技有限责任公司 | After reclaiming light olefin, in oil refinery dry gas, high receipts rate high purity carries hydrogen methods and device |
| CN104607000B (en) * | 2015-02-11 | 2017-09-26 | 中凯化学(大连)有限公司 | C in a kind of oil refinery dry gas2、C3The recovery method of component, light hydrocarbon component and hydrogen |
| CN106831304A (en) * | 2017-04-01 | 2017-06-13 | 天邦膜技术国家工程研究中心有限责任公司 | A method and device for improving the efficiency of catalytic dry gas production of ethylbenzene |
| CN109022033A (en) * | 2017-06-09 | 2018-12-18 | 中石化广州工程有限公司 | A kind of group technology that oil refinery dry gas recycling is isolated |
| CN108011119B (en) * | 2017-12-18 | 2020-12-01 | 陕西省石油化工研究设计院 | Method and system for resource utilization of hydrogen-containing exhaust gas coupled to fuel cell clean power generation |
| CN111467913A (en) * | 2020-03-27 | 2020-07-31 | 大连海奥膜技术有限公司 | Comprehensive recycling process and equipment for refinery tail gas |
| CN116062691A (en) * | 2021-11-01 | 2023-05-05 | 中国石油化工股份有限公司 | Method and system for recycling hydrogen after unsaturated rubber hydrogenation reaction and application thereof |
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2010
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